An eco-friendly one-pot method to synthesize self-assembled palladium nanoclusters using a macrocycle, namely cucurbit[7]uril, in the alkaline medium without employing any special reducing or capping agents and/or external energy at room temperature is described. This greener approach, which utilizes water as a benign solvent and biocompatible cucurbit[7]uril as both reducing and protecting agents, can be applied to synthesize other noble metal nanoparticles such as gold, silver, and platinum. Owing to unique structural arrangement of cucurbit[7]uril, it was possible to prepare palladium nanoclusters of honeycomb-like structure irrespective of the reaction conditions. The honeycomb-like palladium nanoclusters were characterized using transmission electron microscopy (TEM), higher-resolution TEM (HR-TEM), X-ray diffraction (XRD), thermogravimetric analysis (TGA), UV-vis, and FT-IR spectroscopy. Significantly, the synthesized palladium nanoclusters exhibited catalytic activity for the reduction reaction of 4-nitrophenol at room temperature. The approach launched here is easy, green, and user-friendly in contrast to the conventional techniques using polymers or surfactants and harsh reductants. (C) 2014 Elsevier B.V. All rights reserved.