We present our systematic work on the in situ generation of In nanoparticles (NPs) from the reduction of ITO thin films by hydrogen (H2) plasma exposure. In contrast to NP deposition from the vapor phase (i.e., evaporation), the ITO surface can be considered to be a solid reservoir of In atoms thanks to H2 plasma reduction. On one hand, below the In melting temperature, solid In NP formation is governed by the island-growth mode, which is a self-limiting process because the H2 plasma/ITO interaction will be gradually eliminated by the growing In NPs that cover the ITO surface. On the other hand, we show that above the melting temperature In droplets prefer to grow along the grain boundaries on the ITO surface and dramatic coalescence occurs when the growing NPs connect with each other. This growth-connection-coalescence behavior is even strengthened on In/ITO bilayers, where In particles larger than 10 μm can be formed, which are made of evaporated In atoms and in situ released ones. Thanks to this understanding, we manage to disperse dense evaporated In NPs under H2 plasma exposure when inserting an ITO layer between them and substrate like c-Si wafer or glass by modifying the substrate surface chemistry. Further studies are needed for more precise control of this self-assembling method. We expect that our findings are not limited to ITO thin films but could be applicable to various metal NPs generation from the corresponding metal oxide thin films.