Nanomaterials are widely used in electrocatalysts due to their quantum size effect and high utilization efficiency. There are two ways to improve the activity of nanoelectrocatalysts: increasing the number of active sites and improving the inherent activity of each catalytic site. The structure of the catalyst itself can be improved by increasing the number of exposed active sites per unit mass. The high porosity and three-dimensional network structure enable aerogels to have the characteristics of a large specific surface area, exposing many active sites and bringing structural stability through the self-supporting nature of aerogels. Thus, by adjusting the compositions of aerogels, the synergetic effect introduced by alloy elements can be utilized to further improve the single-site activity. In this review, we summarized the basic preparation strategy of aerogels and extended it to the preparation of alloys and special structure aerogels. Moreover, through the eight electrocatalysis cases, the outstanding catalytic performances and broad applicability of aerogel electrocatalysts are emphasized. Finally, we predict the future development of pure metallic aerogel electrocatalysts from the perspective of preparation to application.