Micro-contact printing of self-assembly monolayers (SAMs), i.e., octadecyl-trichlorosilane (OTS) was combined with self limiting atomic layer deposition in order to fabricate the selective deposition of nickel oxide on amorphous Si thin films. The localized nickel species facilitated metal-induced crystallization (MIC) and at later stages, metal-induced lateral crystallization (MILC) in amorphous Si thin films at the elevated temperatures ranging from 500 °C to 550 °C. The uniform coating of SAMs onto amorphous Si thin films was monitored using physical/chemical characterization, i.e., atomic force microscopy, electron microscopy, and Raman spectroscopy. The crystalline feature was found to be superior to the counterpart solid-phase crystallization. The effectiveness of SAMs appears to provide the microscale patterning in addition to the sophisticated control against nickel-species.