Uncontrollable bleeding caused by severe trauma is life-threatening. Therefore, it is of great significance to develop hemostatic materials that meet the rapid hemostasis of wounds. In this study, a water-triggered shape memory carboxylated cellulose nanofiber/sodium alginate/montmorillonite (CNSAMMTCa) composite hemostatic sponge was prepared, which can promote coagulation by concentrating the blood and activating intrinsic pathway. The anisotropic three-dimensional porous structure formed by directional freeze-drying technology improved the performance of composite sponges which showed good prospects in rapid hemostasis. The results showed that CNSAMMTCa composite sponge had good porous structure, water absorption ability, cytocompatibility and blood cell aggregation capacity. Simultaneously, we confirmed that CNSA3MMT2Ca has best coagulation performance in the mouse censored bleeding model and liver rupture bleeding model. Therefore, CNSAMMTCa composite hemostatic sponge is a safe and efficient rapid hemostatic material which is expected to become an alternative material for clinical hemostatic materials.