Visible wavelength surface-enhanced Raman spectroscopy (SERS) has been observed from bovine serum albumin (BSA) using In-InP nanopillars synthesised by Ar gas cluster ion beam sputtering of InP wafers. InP provides a high local refractive index for plasmonic In structures, which increases the wavelength of the In surface plasmon resonance. The Raman scattering signal was determined to be up to 285 times higher for BSA deposited onto In-InP nanopillars when compared with Si wafer substrates. These substrates demonstrate the label-free detection of biomolecules by visible wavelength SERS, without the use of noble metal particles. Surface-enhanced Raman spectroscopy (SERS) utilises the resonant excitation of localised surface plasmons to boost the scattering efficiency from samples containing few or even single molecules 1-3. The technique's usefulness for non-destructive and label-free characterisation has resulted in a large body of research since its discovery in 1974 3,4. Gold and silver nanoparticles have historically been the most often employed SERS substrates due to their strong visible wavelength localised surface plasmon resonance (LSPR) 5,6. However, the price and scarcity of noble metals remains one of the major drawbacks of SERS and, as such, it has been recognised that more cost