The effects of the α-Fe phase on mechanical properties and cracking of laser 3D printing Fe-based bulk metallic glass composites were investigated. The elastic recovery and plasticity index were characterized by nanoindentation. As the volume fraction of the α-Fe phase increases from 23.66% to 52.38%, the elastic modulus of printed samples suddenly drops. The samples exhibit a lower deformation resistance, and the plasticity index increases gradually. When the volume fraction of the α-Fe phase is 67.84%, the interaction between the α-Fe phase and matrix phase is smaller during expansion shrinkage. As a result, cracking is easy to initiate, which leads to the highest crack rate of the printed sample. However, as the volume fraction of the α-Fe phase increases to 83.31%, the hard brittle phase was sandwiched between the α-Fe phases similar to the finger structure plays key role in the plastic deformation. The plastic deformation releases large amounts of stress concentrated at the boundary and suppresses crack formation.