Nickel nanoparticles (Ni NPs) are attracting more and more attention in the field of electrochemistry due to their high conductivity and good catalytic properties. However, Ni NPs are susceptible to corrosion or agglomeration, leading to low stability. In this work, nickel@carbon nanomaterials (Ni@CNS) were prepared by pyrolysis nickel-based metal-organic framework (Ni-MOF) template, and characterized by powder X-ray diffraction (PXRD), transmission electron microscopy, scanning electron microscopy, Brunauer–Emmett–Teller method, and X-ray photoelectron spectroscopy (XPS). The prepared Ni@CNS composite reveals uniform core-shell structure, where the thin carbon shell not only protects the Ni NPs from being corroded, but also accelerates the migration of electrons, so as to promote its sensing performance. Ni@CNS composite presented as a black powder with mesoporous structure. The average size of Ni NPs was about 15.01 nm with a standard deviation of 3.21 nm. The specific surface area of Ni@CNS was as high as 116.12 m2 g[Formula: see text], which is beneficial to increase the effective surface area of the modified electrode. These structural advantages enhance its electrochemical performance toward paracetamol (PA) sensing. The Ni@CNS modified electrode has high sensitivity for quantitative detection of PA. The linear ranges were determined to be 0.570 [Formula: see text]M and 70432 [Formula: see text]M with a low detection limit of 0.028 [Formula: see text]M ([Formula: see text]/[Formula: see text] = 3). In addition, due to its excellent electrochemical performances, the constructed electrode was used to detect PA in real water samples. This work expands the application of Ni- and C-based composites in electrochemistry sensing.