Spin injection across 160 nm thick semi-crystalline Poly(vinylidene fluoride-co-hexafluoropropylene) (PVDF-HFP) is methodically investigated at room temperature in PVDF-HFP/NiFe bilayers and Ag/(NiFe or Co)/PVDF-HFP/NiFe vertical organic spin valves (OSVs) using both the co-planar waveguide ferromagnetic resonance (CPW-FMR: 7-35 GHz) and magnetoresistance (MR) techniques. The structural and microstructural characteristics of PVDF-HFP reveal the formation of mixed non-ferroelectric alpha and ferroelectric beta phases. The spin injection due to the transfer of angular momentum in PVDF-HFP/NiFe is quantified by measuring the spin-mixing conductance (g↑↓) and the enhancement in Gilbert damping (α) parameters from CPW-FMR data. A significant increase inαof 26% andg↑↓of (2.72 ± 0.45) × 1019m-2highlights the efficient spin injection into the PVDF-HFP spacer layer. Further, the MR in OSV structures reveals a room temperature spin injection with a maximum MR of 0.278 ± 0.006% for Ag/Co/PVDF-HFP/NiFe and 0.349 ± 0.039% for the Ag/NiFe/PVDF-HFP/NiFe devices. Furthermore, the spin injection processes are discussed w.r.t to bias voltages, interfaces and microwave frequencies.