Inspired by the self-recoverability ability of organisms, various self-healing materials have been developed. However, most reinforced fillers are faced with the problem that mechanical strength and self-healing efficiency of materials cannot be improved simultaneously. Here we first prepared new polysiloxane-polyurea (PDMS-PU) and used it as matrix resin to prepare cellulose nanofiber (CNF)/PDMS-PU composite materials with high mechanical properties. CNFs increased the tensile strength of PDMS-PU by 38.87 % and CNF/PDMS-PU composite materials maintained the great bending resistance, transparency and reprocessing properties of PDMS-PU. Moreover, the introduction of CNFs did not reduce the self-healing efficiency of PDMS-PU, and PDMS-PU containing disulfide bonds with CNF content of 1 % (CNF/PDMS-IPDI-S-1 %) with healing efficiency of 95.58 %, and the tensile strength after three recycling processing was still as high as 92.55 % of the original. CNFs reinforced PDMS-PU composite materials are expected to replace PDMS materials in advanced engineering fields that require high strength durability and good formability.