Bio-derived ketones can be converted to aviation fuel by aldol self-condensation followed by hydrodeoxygenation. Anionic clays, particularly hydrotalcites (HT), have a high density of base sites generating higher condensation conversion and yield compared to other catalysts. In this work, calcined, air plasma treated, and rehydrated Mg/Al-hydrotalcite on granular activated carbon (GAC) catalyst were synthesized and a series of self and cross condensation reactions with acetone (AC) and cyclopentanone (CP) were studied. The best conversion was 37% for self-condensation of AC by using sonicated rehydrated calcined HT at 500 °C supported by GAC compared to 28% by using unsupported HT calcined at 500 °C. For self-condensation of CP, 61% conversion was obtained by using air plasma treated HT calcined at 500 °C supported by GAC versus 42% by using calcined HT at 500 °C. For cross-condensation of AC and CP the conversion was 71.5% by using sonicated rehydrated calcined HT at 500 °C supported by GAC versus 67% by using unsupported HT calcined at 500 °C. The solid base catalyst supported by GAC could potentially be recoverable, reusable, and used in continuous processing.