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This study reports a simple new technique for the preparation of novel hexagonal-shaped mixed metal oxides (MMO) nanorods using Zn/Al-layered double hydroxide (LDH) as a precursor for dye-sensitized solar cell (DSSC) application. The effect of the Zn to Al molar ratio demonstrated a sound correlation between the obtained nanorods’ diameter and the fabricated DSSCs efficiency. Additionally, the optical behavior of the fabricated MMO film as well as the absorption enhancement due to the utilized dye are also demonstrated; a cut-off phenomenon at around 376 nm corresponds to the attained hexagonal nanorods. The open-circuit voltage augmented noticeably from 0.6 to 0.64 V alongside an increase in the diameter of nanorods from 64 to 80 nm. The results indicated that an increment in the diameter of the nanorods is desirable due to the enhanced surface area through which a higher amount of dye N719 was loaded (0.35 mM/cm2). This, in turn, expedited the transport of electrons within the MMO matrix resulting in an advanced short-circuit current. Of the devices fabricated, ZA-8 exhibited the highest fill factor and efficiency of 0.37% and 0.69%, respectively, because of its boosted short-circuit current and open-circuit voltage.