Wettability is a key parameter for optimizing the residual oil recovery from geological rock formations and it provides a path for improved oil recovery and geo-storage of energy. Thus, the key motive behind wettability alteration from hydrophobic to hydrophilic is to enhance the oil productivity. Thus, this work concentrates on Sui main limestone reservoir core samples’ wettability alteration (altering their surface wetting behavior from an oil-wet to water-wet state) for enhanced oil recovery. Hence, we examine the effectiveness of alumina nanofluid as well as a new chemical methyl blue to alter the wettability. Methyl blue is released on a large scale from various industries, i.e., pharma, textile, and food industries, which is a key environmental concern; subsequently, it contaminates the water table. Hence, the study explores the effects of MB and alumina nanofluid on wettability. The effect of nanofluids formulated via dispersing the alumina nanoparticles in aqueous solutions at various concentrations (0. 0.05, 0.3, 0.50, 0.75, and 1.0 wt. %) were tested for wettability modifications under different physio-thermal conditions. Subsequently, the wettability change was examined for these samples treated with different concentrations of MB (10, 15, 30, 50, and 100 mg/L) for 7 days at two different temperatures (25 and 50 °C). The results show that the hydrophobicity of the SML carbonate rock significantly reverses while treating with alumina nanofluids and MB. Thus, the wettability modification/reversal via the treatment of MB and alumina nanofluids can be an effective mechanism for hydrogen injections and EOR processes.