Globally increasing concerns have been raised on the high energy consumption and greenhouse gas emissions in conventional municipal wastewater treatment processes over the past decades. In this study, a self-sustaining synergetic microalgal-bacterial granular sludge process was thus developed to address these challenges. The results showed that the microalgal-bacterial granular sludge process was capable of removing 92.69%, 96.84% and 87.16% of influent organics, ammonia and phosphorus under non-aeration conditions over a short time of 6 h. The effluent could meet the increasingly stringent discharge standards in many countries worldwide. A tight synergetic interrelationship effect between microalgae and bacteria in granules was essential for such excellent process performance. The stoichiometric and functional genes analyses further revealed that most of organic matter and nutrients were removed through microalgal and bacterial assimilations. Moreover, it was found that there existed a desirable distribution of functional species of microalgae and bacteria in microalgal-bacterial granules, which appeared to be essential for the self-sustaining synergetic reactions and stability of microalgal-bacterial granules. Consequently, this work may offer a promising engineering alternative with great potential to achieve energy-efficient and environmentally sustainable municipal wastewater treatment.