A new cellulose nanocrystal–reduced graphene oxide (CNC–rGO) nanocomposite was successfully used for mediatorless electrochemical sensing of methyl paraben (MP). Fourier-transform infrared spectroscopy (FTIR) and field-emission scanning electron microscopy (FESEM) studies confirmed the formation of the CNC–rGO nanocomposite. Cyclic voltammetry (CV) studies of the nanocomposite showed quasi-reversible redox behavior. Differential pulse voltammetry (DPV) was employed for the sensor optimization. Under optimized conditions, the sensor demonstrated a linear calibration curve in the range of 2 × 10−4–9 × 10−4 M with a limit of detection (LOD) of 1 × 10−4 M. The MP sensor showed good reproducibility with a relative standard deviation (RSD) of about 8.20%. The sensor also exhibited good stability and repeatability toward MP determinations. Analysis of MP in cream samples showed recovery percentages between 83% and 106%. Advantages of this sensor are the possibility for the determination of higher concentrations of MP when compared with most other reported sensors for MP. The CNC–rGO nanocomposite-based sensor also depicted good reproducibility and reusability compared to the rGO-based sensor. Furthermore, the CNC–rGO nanocomposite sensor showed good selectivity toward MP with little interference from easily oxidizable species such as ascorbic acid.