VO2/CoFe2O4 nanoparticle composites were synthesized by hydrothermal method combined with annealing treatment. The nanocomposites consist of quasi-spherical nanoparticles with an average size of about 70 nm. The thermochromic properties of the nanocomposite films can be modulated by changing film thickness and the content of CoFe2O4 in the nanocomposites. The band gap of the VO2/CoFe2O4 nanocomposites increases with increasing CoFe2O4 additive content. The introduction of CoFe2O4 into VO2 matrix can not only lower the phase transition temperature, but also optimize the luminous transmittance and solar modulation ability of the VO2/CoFe2O4 nanocomposites as well. Our findings demonstrate a promising avenue in constructing VO2-based smart films with excellent thermochromic performance.