One of the major challenges in tissue engineering is to engineer biomaterial scaffolds with desirable gradients for the regeneration of composite tissues. Here we propose a unique electrospinning strategy to fabricate nanofibrous scaffolds with both structure and material composition gradients. The results demonstrate that the microstructural organization of nanofibers gradually changed from random to aligned patterns. Nanoparticles like nanohydroxyapatite (nano-HA) were encapsulated into these nanofibers and nano-HA content in the electrospun scaffolds gradually altered in a similar gradient manner to structural organization. This simple yet versatile method might be useful to engineer graded tissues by flexibly generating tissue-specific structure and material gradients. (c) 2014 Elsevier B.V. All rights reserved.