Electrochemical CO2 reduction reaction (eCO2RR) is a promising route for removal of CO2 from the atmosphere and transforming it into value-added products. The development of new and efficient catalysts plays a vital role in this regard. Here a combination of carbon grafting and bimetallic metal aerogel is presented as a catalyst for eCO2RR. The grafted surface plays an essential function in assembling the catalyst on the carbon cloth (CC) surface as a supported catalyst. Herein, we describe the use of para-aminothiophenol (p-TP) as a grafting agent combined with diazonium chemistry to fix a metallic aerogel catalyst on CC as support. The silver, palladium and bi-metallic silver-palladium aerogels (Ag-p-TP, Pd-p-TP, and AgPd-p-TP) anchored onto the surface of CC yielding the corresponding surface-bound materials were used for testing the electrochemical reduction of CO2. The mono-metallic Ag carbon cloth (Ag-p-TP/CC) exhibited the ability in reducing CO2 to CO with moderate Faradaic efficiency (FE) of 74 % in 0.1 M, NaHCO3 electrolyte at pH = 7.5. The bimetallic AgPd-p-TP-CC further enhanced the Faradaic efficiency for CO formation to 88.7 %, with an unexpectedly low onset potential of −0.09 V vs. RHE. Surprisingly, formate was identified to be the liquid product when Pd-p-TP-CC and AgPd-p-TP-CC were used, with maximal FEformate of 19.0 % and 25.7 % at −1.0 V vs. RHE, respectively. In contrast, CC lacking the chemical grafting that allows immobilization of the metal aerogel (Ag-Pd/CC) exhibits lower FEco% for eCO2RR, highlighting the importance of this chemical modification of the carbon cloth surface. Diazonium chemistry coupled with metal aerogels is a new approach to generating surface-bound catalysts for the effective reduction of CO2.