In this paper, we present a novel strategy, named Synchronous One-Pot (SOP) synthesis, to prepare gold nanoparticles (AuNPs) with a diameter of 2 nm incorporated in self-assembled organic spheres with a diameter around 60 nm (denoted as NPAs). Merits of this method include: (1) self-assembly of the organic component (calix[6]biscrown TAC) into spheres and the reduction of chloroauric acid (HAuCl4) take place simultaneously; (2) preparation combining UV irradiation and formaldehyde addition reduces the size and homogenizes the distribution of the resultant AuNPs within the TAC spheres. (3) Obtained material NPA gives attractive catalytic property to hydrogenation reaction. (C) 2012 Elsevier Inc. All rights reserved.