Since the past two decades, ultrafast two-dimensional electronic spectroscopy (2DES) has made remarkable progress, and it plays a pivotal tool in unraveling population and coherent dynamics in photosynthesis, photovoltaic, and low-dimensional materials. This review presents a comprehensive overview of the progress in 2DES, with a focus on its ability to expand spectral windows and dimensions. Furthermore, it examines the current challenges and future directions of this field. From a technical perspective, a key bottleneck preventing the wide application of 2DES is the need to overcome experimental hurdles and develop sophisticated multispectral data analysis methods. In cutting-edge research, a crucial question centers on the development of novel 2DES techniques to effectively probe and disentangle various processes within coherent dynamics and polaritonic systems.