Electrospun carbon and polymer nanofibers were studied as possible substrates for surface–enhanced laser desorption ionization. Using the carbon nanofibers, organic polymers could be observed using SALDI ionization with much improved S/N and reproducibility compared to using the conventional stainless steel substrate. Matrix Assisted Laser Desorption Ionization often has challenges with matrix interfering with the analysis of low molecular weight compounds; carbon nanofiber based substrates allow clean high signal/ noise spectra of low molecular weight compounds to be readily obtained. Detection limits as low as 400 attmol were observed of angiotensin I using carbon nanofiber based supports with matrix enhanced-SALDI conditions