The use of nitrogen (N) fertilizers increases crop yield, but the accumulation of residual N in agricultural soils poses significant environmental risks. Improving the N use efficiency (NUE) of crops can help reduce N pollution. While nanomaterials have been shown to enhance crop agronomic traits, more research is needed to clarify the regulatory mechanisms involved. In this study, foliar spraying of carbon dots (CDs, 1 mg·mL−1) derived from Salvia miltiorrhiza increased the activity of plasma membrane H+-ATPase in Arabidopsis thaliana roots, promoting the uptake, transport, and assimilation of NO3- and NH4+. The upregulation of N metabolism-related genes, such as AtAMTs and AtNRTs, was also observed in A. thaliana roots. Transcriptome analysis suggested that this regulatory effect is mediated by the shoot-to-root mobile polypeptide CEPD1 (C-terminally encoded peptide DOWNSTREAM 1) signaling pathway. Additionally, foliar application of CDs increased the NUE of sweetpotato (Ipomoea batatas (L.) Lam.) from 2.5% to 8.1%. The upregulation of genes such as CEPD1 in leaves was observed following CDs application under different N conditions. Finally, foliar spraying of CDs significantly increased field yield and enhanced tolerance to low N stress in sweetpotato. Overall, this study demonstrated that foliar application of CDs improved NUE in plants through CEPD1-dependent signaling.