The magnetic anisotropy is decreased with increasing temperature in normal magnetic materials, which is harmful to the thermal stability of magnetic devices. Here, we report the realization of positive temperature coefficient of magnetic anisotropy in a novel composite combining β-phase polyvinylidene fluoride (PVDF) with magnetostrictive materials (magnetostrictive film/PVDF bilayer structure). We ascribe the enhanced magnetic anisotropy of the magnetic film at elevated temperature to the strain-induced anisotropy resulting from the anisotropic thermal expansion of the β-phase PVDF. The simulation based on modified Stoner-Wohlfarth model and the ferromagnetic resonance measurements confirms our results. The positive temperature coefficient of magnetic anisotropy is estimated to be 1.1 × 10(2) J m(-3) K(-1). Preparing the composite at low temperature can enlarge the temperature range where it shows the positive temperature coefficient of magnetic anisotropy. The present results may help to design magnetic devices with improved thermal stability and enhanced performance.