Supplemental Materials The alloy studied was Ti-5.at% Al, loaded in double slip orientation. For micron/submicron samples, the pillars had square cross sections with the edge length (L) or diameter (d) ranging from 5.0 μm to 150 nm, and an aspect ratio of ~2. In situ Transmission Electron Microscopy (TEM) tensile samples had width around 200 nm. All samples were cut out from a bulk single crystal with well defined orientation determined using the method described in previous work (10-11). The samples were loaded in approximately the “double slip” orientation, as two equivalent prismatic slip systems, (01-10)[2-1-10] and (-1100)[11-20] are expected to have the highest propensity to be activated (1,2). Larger samples were tested in compression in a MTS Nanoindenter XP device outfitted with a flat punch diamond tip, at a nominal axial strain rate ~ 110-4s-1 at room temperature. Cross-sectional TEM samples of these deformed pillars were produced by Focus Ion Beam (FIB) using the “lift out” method and analyzed under a JEOL 3010 TEM. In the same TEM, samples with sizes below 200 nm were compressed or pulled by using a Hysitron Picoindenter in the method that has been described before (3,4). All mechanical tests were under displacementcontrolled mode. Further thinning was performed in a Triple-beam Focus Ion Beam with final milling by using 2KV Ar+ source to reduce the FIB damage, for atomic resolution imaging of the microstructure of the deformed samples in a Philips CM 300 high-resolution TEM (HRTEM). We first note that slip systems 1/3(01-10)[2-1-10] and 1/3(-1100)[11-20] on prismatic planes would be the first ones to be activated. Dislocations from these two slip systems will intersect with each other and form junctions, and in bulk samples the large number of junctions formed will produce a rather robust dislocation network that leads to stain hardening and stable flow (2). This phenomenon can be also observed in our micron-sized samples. Figure S1a shows the interlaced strain field produced by the dislocation network in one micron-sized pillar (the two dislocation types are marked). However, with continued deformation and rising stresses the pinning at the limited number of junctions eventually loses its grip, such that the dislocations eventually pulls away in an avalanche, producing uncontrollable strain bursts (Fig. 1a in main text) in lieu of sustainable/stable plastic strain. Cross-sectional TEM of the micron-sized deformed samples revealed a large number of “U” and “H” shaped dislocations. Examples are shown in Figure S1b and Fig. 3a in the main text. Different from that in bulk samples, it appears that the interaction and tangling between dislocations is weaker in our small samples, due to the limited chances for the dislocations to intersect and form junctions in the small volume. A dislocation would encounter and be pinned by only a couple of dislocations from the other slip system, leaving two long single arms on both ends. Once the applied stress is enough to overcome the barrier from the single pinning point at the dislocations intersection, the arms could escape and continue to slip until leaving the sample from the surface. In other words, the cross-sectional TEM observations in Figure S1b indicate no multiple-pinned segments left behind, consistent with very limited number of junctions. As such, the dislocation groups resulting from deformation can easily disintegrate, resulting in collective dislocation avalanche, or a pronounced strain burst, in a way similar to those in face centered cubic (FCC) and body centered cubic (BCC) pillars. With decreasing sample size, the dislocations became even less organized and retained. Figure S1 (a) Typical HRTEM image that shows the interlaced strain field produced by the dislocation network in one micron-sized pillar (the two dislocation types are marked). (b) The TEM image of the cross section of one micro-pillar after deformation. “U” and “H” shaped dislocations are marked. g=[4-2-20]. In addition, according to the E. A. Metzbower’s work (5), the stacking fault probability a is the function of the aluminum content CAl as a = 0.003exp(0.133CAl), here CAl is the weight percent (wt pct). It is also reported that the stacking faults energy is assumed to have an inverse relationship (6) with stacking fault probability a as = K/a. K can be determined to be 0.9 mJ/m2 by the pure Ti with = 300 mJ/m2, a = 0.003. Thus, with our present sample Ti-5.0at% of CAl = 2.9 wt pct, the calculated stacking faults energy is assuming to be decreased to 204 mJ/m2. Although the stacking faults of Ti-5.0at% alloy is decreased compared to the pure Ti, it is still quite high in comparison with some other metals such as Ag (22 mJ/m2) (7), Cu (55 mJ/m2) (7) and Al (166 mJ/m2) (8). Reference: 1 X. Tan, H. Gu, C. Laird, N.D.H. Munroe, Metallurgical and Materials Transactions A 29A, 507(1998). 2 L. Xiao, Y. Umakoshiz, Philosophical Magazine, 82, 2379(2002). 3 Q. Yu, Z.W. Shan, J. Li, X. X. Huang, L. Xiao, J. Sun, E. Ma, Nature, 351, 335(2010). 4 D. Kiener, A.M. Minor, Nanoletters, 11, 3816(2011). 5 E. A. Metzbower, Metall. Trans., 2, 3099 (1971). 6 R.P. Adler, H.M. Otte, C.N.J. Wagner, Metall. Trans., 1, 2375 (1970). 7 P. C. J. Gallagher, Metall. Trans., 1, 2429 (1970). 8 L. E. Murr, Acta Metall., 21, 791 (1973).