Manipulation of magnetic moments through spin transport is determined by the effective spin mixing conductance g eff ↑↓ in the ferromagnetic metal/heavy metal heterostructure. Magnetization dynamics detection and evaluation of the Gilbert damping constant α is usually employed to estimate g eff ↑↓. An all-optical pump-probe method is a powerful method for investigating α with high accuracy because an extrinsic contribution on α can be suppressed at a high precession frequency with an increasing external magnetic field. A large voltage signal was recently observed in half-metallic Heusler alloy Co2MnSi thin film due to spin current injection; however, that voltage signal may also include contributions from thermal effect and spin Hall angle in the heavy metal layer. In this study, a large enhancement of α was observed in Co2MnSi/Pt heterostructure by using the all-optical method. g eff ↑↓ for Co2MnSi/Pt was 2 times larger than that for Fe/Pt. This large g eff ↑↓ is promising for spintronic device applications.