In this study, crystallization was effectively suppressed in Al-based metallic glasses (Al-MGs) during pulverization by cryo-milling by applying an extremely low processing temperature and using a surfactant. Before Al-MGs can be used as an additive in Ag paste for solar cells, the particle sizes of the Al-MGs must be reduced by milling. However, during the ball milling process crystallization of the Al-MG is a problem. Once the Al-MG is crystallized, they no longer exhibit glass-like behavior, such as thermoplastic deformation, which is critical to decrease the electrical resistance of the Ag electrode. The main reason for crystallization during the ball milling process is the heat generated by collisions between the particles and the balls, or between the particles. Once the heat reaches the crystallization temperature of the Al-MGs, they start crystallization. Another reason for the crystallization is agglomeration of the particles. If the initially fed particles become severely agglomerated, they coalesce instead of being pulverized during the milling. The coalesced particles experience more collisions and finally crystallize. In this study, the heat generated during milling was suppressed by using cryo-milling with liquid-nitrogen, which was regularly fed into the milling jar. Also, the MG powders were dispersed using a surfactant before milling, so that the problem of agglomeration was resolved. Cryo-milling with the surfactant led to D50 = 10 um after 6 h milling, and we finally achieved a specific contact resistance of 0.22 mΩcm2 and electrical resistivity of 2.81 μΩcm using the milled MG particles.