The effect of direct current (dc) substrate bias on the promotion of nanocrystallization in Si network has been studied, specifically within He-diluted SiH4 plasma in radio frequency (RF)-plasma-enhanced chemical vapor deposition. In view of organizing nanocrystallinity, controlled transmission of energy to the growing surface is needed and that is obtainable from metastable helium (He*) bombardment and, in particular, ionic helium (He+) bombardment under negative substrate bias. The structural morphology has been adequately regulated to a homogeneous network restraining from an exclusive columnar structure that is coherent to low-temperature growth. Notable improvements in the film quality in terms of enhanced crystallinity with low hydrogen content as well as reduced incubation volume, bulk void, and surface roughness have been demonstrated, even at low substrate temperature and low RF power. Use of appropriate dc substrate-bias has been identified as a supplementary parameter efficiently organizing the growth, making it more device-friendly.