The Quartz Crystal Microbalance (QCM) plays a crucial role as an electronic cornerstone in gas sensor development, capable of detecting minute mass alterations on its quartz crystal resonator triggered by gas molecule adsorption or desorption. In this study, we adopt the QCM dip-coat technique, involving the application of layers comprising pairs of calix[6]arene and 4-tert-Butylcalix[4]arene to enhance sensor sensitivity. Results demonstrate that employing three pairs significantly boosts gas vapor detection compared to using two or one pair. Sensor sensitivity is validated through the testing of various concentrations of Volatile Organic Compounds (VOCs) gases, revealing a direct correlation between gas dilution and impedance levels. Observed gas detection trend indicate that toluene vapor induces higher impedance than acetone and ethanol due to its greater molecular weight. Toluene’s higher molecular weight fosters stronger interactions with the quartz surface, resulting in more pronounced frequency shifts and higher impedance readings. Moreover, our findings align with the Sauerbrey Equation, confirming the reliability and accuracy of the QCM-based gas sensor developed in this study. The incorporation of calix[6]arene and 4-tert-butylcalix[4]arene in the QCM dip-coat technique enhances gas molecule entrapment by providing increased surface area, selective binding, synergistic effects, and stabilization, consequently amplifying sensor sensitivity and performance.