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• Size-tunable monodisperse Pd nanocrystals were prepared in a rotating packed bed. • They were adopted as pseudohomogeneous catalyst for nitrobenzene (NB) reduction. • 2.6 nm Pd nanocrystals displayed excellent catalytic property and good stability. • The obtained catalytic kinetics data confirm to the Langmuir-Hinshelwood model well. • DFT calculation was used to study the adsorption of NB on the surface of catalyst. Nitrobenzene (NB) reduction is an important catalytic reaction, which is commonly performed in aqueous medium mainly with heterogeneous catalysts. In this work, highly stable aqueous nanodispersions of Pd nanocrystals with a tunable average size between 2 and 11 nm are conveniently prepared in a high-gravity rotating packed bed (RPB) reactor, and firstly serve as a pseudohomogeneous catalyst for NB reduction. As compared to a conventional stirred tank reactor (STR), the product prepared in the RPB reactor has a more uniform particle size. More importantly, the reaction time can be greatly shortened from 3 min (STR) to 1 s (RPB), thereby realizing a continuous preparation. This Pd pseudohomogeneous catalyst displays a significantly size-dependent catalytic activity and a good stability performance. Ultra-small 2.6 nm Pd nanocrystals have a reaction rate five times as fast as 10.1 nm counterpart. The obtained kinetics data confirm to the Langmuir-Hinshelwood model well, having a small error of <10%. Furthermore, the adsorption behavior of NB molecules on the surface of Pd nanocrystals was also studied with density functional theory (DFT) calculation. Since the processing capacity of the used lab-scale RPB reached 44.2 g/h, this route may offer a general platform for mass production of monodisperse nanocrystals as pseudohomogeneous catalyst for highly efficient catalysis. [ABSTRACT FROM AUTHOR]