A straightforward method, which is termed novel handspinning, is reported for producing uniaxially aligned sPP nanofibers. As demonstrated by SEM analysis, the morphologies of handspun sPP nanofibers are strongly dependent upon the processing conditions such as spinning method and solvent system. Compared to the normal electrospun sPP nanofibers, the handspun sPP nanofibers show smoother morphologies. FT-IR analysis demonstrates a significant difference in polymer chain conformation between the handspun and electrospun sPP nanofibers. Moreover, interestingly, the handspun sPP single nanofibers show higher Young's modulus and tensile strength than electrospun sPP single nanofibers.