Amino-terminated silane compound modification was wet--processed on a silicon wafer using four different solvents to investigate the property of the self-assembled monolayer (SAM) and its influence on the adhesion of electroless deposited nickel-phosphorus (Ni-P) films. Analyzed by various tools including dynamic light scattering, the atomic force microscope, X-ray photoelectron spectroscopy, inductively coupled plasma with mass spectroscopy, a proper link between the processing solvent and SAM quality is established. It is found that at least the chemical compatibility, the polarity, and the acidity of solvents can affect the final morphology of the resultant SAM. Unlike toluene and ethanol that are most frequently chosen in literature, we conclude that isopropyl alcohol (IPA) is a superior solvent for amino terminated silane compounds. Owing to the good SAM quality formed in IPA, the adhesion of electroless deposited Ni-P films is largely strengthened, even as high as the bulk strength of silicon wafers.