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In this paper, the modified embedded atom method (MEAM) potential function was introduced to study the solid-phase sintering (SPS) mechanism and the mechanical properties of Fe9.5Co (at%) elastocaloric refrigeration alloys through molecular dynamics (MD) simulations. The analysis of the energy field showed that the mechanism of SPS was the free surface annihilation (FSA) and the re-bonding process of atoms on the two surfaces. The energy released by FSA per unit area was calculated to be 1.89eV/Å2. In addition, the analysis of the sintering process parameters further confirmed the SPS mechanism. The evaluation of the mechanical properties of the alloy showed that mechanical properties of the Fe9.5Co (at %) alloy were greatly affected by the strain rate and temperature. This work provided theoretical guidance for the preparation of Fe9.5Co (at %) elastocaloric refrigeration alloys and laid a foundation for the study of elastic thermal effects.