Carbon quantum dots (CQDs) with fluorescence emission have been widely studied for versatile applications, but facile tunability of the spectral properties of CQDs by doping remains to be further explored. Herein, employing lanthanide ion Eu3+ as a dopant and activator, a simple and efficient synthesis route for pure CQDs and Eu-CQDs was demonstrated using N, N-dimethylformamide, oleic acid, and oleylamine as precursors for carbon sources. In comparison, with the popular citric acid precursor, the as-prepared CQDs and Eu-CQDs exhibited an obviously smaller particle size (1.72 ± 0.29 nm) and a more uniform distribution. Through systematic optimization of Eu3+ doping for the Eu-CQD system, colorful light emissions in the visible range were first realized under excitation of ultraviolet (UV) ∼360 nm for promising application of UV-triggered light-emitting diodes. Most interestingly, this Eu-CQD solution with UV-excited colorful light emissions was utilized as a visual pH sensor, experimentally featuring good repeatabilities and stabilities (pH values switching between 7 and 14). Besides, the Eu-CQD solution exhibited highly sensitive detection characteristics for Co (II) ions. Due to the spectral overlapping, the quenching efficiency is as high as 96.3%, and the detection limit is obtained as 0.139 μM, which is much lower than the maximum concentration of Co (II) in the drinking water permitted by WHO. All of these relevant results significantly demonstrate the great potential of lanthanide doping in the multifunctionalization of CQDs for certain emerging applications like lighting, sensing, and detection.