Crystallization employing an N-(2-aminoethyl)-3-aminopropyltrimethoxysilane self-assembled monolayer (AEAPS-SAM) to coordinate Ni metal catalyst was found to produce large grain poly-Si. A small concentration of Ni could be deposited controllably onto an AEAPS-SAM covered with Si by immersing it in Ni solution for 1–60min. Larger grains and a lower Ni concentration in the poly-Si could be obtained by shorter immersion. Immersion for 1min produced grains, as large as 47μm and a Ni concentration as low as 7.4×1018atoms/cm3. A poly-Si thin-film transistor fabricated with AEAPS-SAM poly-Si of 1min immersion had a field-effect mobility of 98cm2/(Vs), which is one order of magnitude higher than that of a thin-film transistor fabricated without the AEAPS-SAM treatment.