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A homogeneous electrochemical deposition method was used in this study of CdAl nanoparticles onto CP fibers at −1.1, −1.2, −1.3, and −1.4 V vs. RHE to prepare highly active, selective, and stable CdAl-LDHs nanocatalysts. The electrochemically deposited materials exhibited extremely high CO selectivity during CO 2 RR, with the CO FE reaching 99.71% at −1.6 V vs. RHE and a partial current density of 22.13 mA cm−2. The CdAl-LDHs maintained excellent CO FE along with high CO partial current density. Remarkably, the CdAl-LDHs demonstrated outstanding electrochemical performance that exceeded most of the reported CO 2 reduction to CO electrocatalysts, maintaining stable electrocatalytic performance for more than 30 h with the FE remaining stable at about 99% and a current density at 10.05 mA cm−2 with little decay. [Display omitted] • CdAl nanoparticles with high activity, selectivity and stability were directly deposited on CP fibers by electrochemical deposition method. • The materials prepared by electrochemical deposition exhibit extremely high CO selectivity in the CO 2 RR process, with Faraday efficiency up to 99.71 %. • CdAl-LDHs can maintain the electrocatalytic performance for more than 30 h, and in this process, and the Faraday efficiency can be stable at about 99 %. Layered bimetallic hydroxides are at the forefront of current research in electrocatalytic materials. Although there is considerable research on various bimetallic hydroxides, the study of bimetallic hydroxides for electrocatalytic reduction of carbon dioxide is limited. In this paper, cadmium-aluminum layered bimetallic hydroxide nanoparticles (CdAl-LDHs) were prepared using a simple electrochemical deposition method. The prepared CdAl-LDHs was characterized in detail, and its potential application as an electrocatalyst was discussed. CdAl-LDHs prepared using different methods showed different selectivity in the electrocatalytic reduction of CO 2 to CO. The nanomaterial exhibits excellent CO selectivity in a reaction chamber using 2 %-BMIM(PF 6)(1-butyl-3-methylimidazolium hexafluorophosphate)/DMF(N-N dimethyl formamide) as the electrolyte. The CdAl-LDHs prepared by electrochemical deposition exhibited a maximum CO partial current density of 22.13 mA cm−2 with a remarkable CO Faraday efficiency (FE) of 99.71 %, which is comparable to or even higher than that of noble metal catalysts. This high selectivity for CO indicates its potential as an alternative to expensive noble metal catalysts. Moreover, the catalyst demonstrated high stability over 30 h of continuous operation with stable FE of around 99 % and a current density of around 10.5 mA cm−2, with minimal degradation during the entire reaction cycle. In addition, the catalyst showed a low HER current density of less than 0.1 mA cm−2 at all tested potentials, indicating that the catalyst maintains a high level of CO 2 conversion over the entire range of tested potentials. This suggests its great potential for industrial applications. [ABSTRACT FROM AUTHOR]