In order to promote low-carbon sustainable operational management of the wastewater treatment plants (WWTPs), automatic control and optimal operation technologies, which devote to improving effluent quality, operational costs and greenhouse gas (GHG) emissions, have flourished in recent years. There is no consensus on the design procedure for optimal control/operation of sustainable WWTPs. In this review, we summarize recent researches on developing control and optimization strategies for GHG mitigation in WWTPs. Faced with the fact that direct carbon dioxide (CO2) emissions (considered biological origin) are generally not included in the carbon footprint of WWTPs, direct emissions (nitrous oxide (N2O), methane (CH4)) and indirect emissions are paid much attention. Firstly, the plant-wide models with GHG dynamic simulation, which are employed to design and evaluate the automatic control schemes as well as representative studies on identifying key factors affecting GHG emissions or comprehensive performance are outlined. Then, both traditional and advanced control methods commonly used in GHG mitigation are reviewed in detail, followed by the multi-objective optimization practices of control/operational parameters. Based on the mentioned control and (or) optimization strategies, a novel design framework for the optimal control/operation of sustainable WWTPs is proposed. The findings and design framework proposed in the paper will provide guidance for GHG mitigation and sustainable operation in WWTPs. It is foreseeable that more accurate and appropriate plant-wide models together with flexible control methods and intelligent optimization strategies will be developed to satisfy the upgrading requirements of WWTPs in the future.