The combination of xanthine oxidase inhibitor febuxostat (FBX) with acetaminophen (ACE) is widely used in the treatment of gout. A rapid, simple, selective, and precise densitometric method was developed and validated for the simultaneous estimation of FBX–ACE mixture in a synthetic binary mixture and in their pharmaceutical dosage forms. The method employed thin-layer chromatography (TLC) aluminum plates precoated with silica gel G 60 F254 as the stationary phase using chloroform-methanol-cyclohexane-acetic acid 96% (7:1:1:0.1, v/v) as the mobile phase. The optimized mobile phase selected for development gave compact bands (Rf values were 0.65 and 0.46 for FBX and ACE, respectively). Spectrodensitometric scanning integration was performed using dual-wavelength detection at 320 and 250 nm for FBX and ACE, respectively. The linear regression data for the calibration plots showed excellent linear relationship (r = 0.9997 and 0.9992 for FBX and ACE, respectively). The method was validated for precision, accuracy, robustness, and recovery. The limits of detection and quantification were calculated. The statistical analysis proved that the method is reproducible and selective for the estimation of this binary mixture.