A versatile synthesis procedure for composite nanofibers, combining electrospinning and atomic layer deposition (ALD), is presented. Both solid core/sheath nanofibers and nanoparticle loaded nanotubes can be made, depending on the order of calcination of the electrospun fiber and the ALD process. Magnetic and photocatalytic nanofibers prepared this way can be recycled readily by collecting with a magnet.