The efficacy of neurofeedback is a point of great controversy, because a certain proportion of users cannot properly regulate their brain activities and thereby fail to benefit from neurofeedback. To address the neurofeedback inefficacy problem, the present study is aimed to design and implement a new neurofeedback system that can more effectively and consistently regulate users’ brain activities than the conventional way of training users to voluntarily regulate brain activities. The new neurofeedback system delivers external visual stimuli continuously at a specific alpha phase, which is real-time decoded from ongoing alpha wave, to regulate the alpha wave. Experimental results show that the proposed training-free externally-regulated neurofeedback (ER-NF) system can achieve consistent (effective in almost all sessions for almost all users), flexible (either increasing or decreasing peak alpha frequency and alpha power), and immediate (taking or losing effect immediately after stimulation is on or off) modulation effects on alpha wave. Therefore, the ER-NF system holds great potential to be able to more reliably and flexibly modulate cognition and behavior.