Metal organic films onto the solid surface have been successfully assembled through Layer-by-Layer (LbL) deposition methods. The organic ligand isonicotinic acid (3-pyridylmethylene) hydrazide containing pyridine groups was chosen to act as a useful building unit, and K2PdCL4 was used as the precursor for the films preparation. UV-vis spectra, transmission electron microscopy (TEM), atomic force microscopy (AFM), and inductively coupled plasma optical emission spectrometry (ICP-OES) were applied to understand the growth process of the resulting LbL multilayers. The LbL films with 10 layers (denoted as (Pd-ligand)(10)) were further applied as catalysts for the hydrogenation of nitroarenes. It is worth mentioning that our films catalyst is convenient to recycle and possesses good reusability.