In this work, a series of Ga1-xAlxFeO3 (x = 0, 0.1, 0.2, 0.5) nanoparticles was prepared by a modified Pechini method. The influence of Al doping at the Ga site on the structural, magnetic, and magnetodielectric (MD) properties of GaFeO3 nanoparticles was studied. The X-ray diffraction pattern analysis using the Rietveld refinement method indicated that all samples have an orthorhombic structure with Pc2(1)n space group and the value of lattice parameters decrease systematically with increasing Al concentration. Interestingly, the magnetic characterization indicated that with increasing Al-content up to 0.5, the ferrimagnetic transition temperature (T-C) increases from 310 to 350 K. It is also found that magnetic hysteresis curves measured below T-C exhibit two-phase-like magnetic behavior consisting of hard and soft magnetic phases. Moreover, the simultaneous improvement of magnetic behavior and MD effect of Al-doped GaFeO3 samples are prominent candidates for the applications of room temperature multiferroic devices. (c) 2020 Author(s). All article content, except where otherwise noted, is licensed under a Creative Commons Attribution (CC BY) license (http://creativecommons.org/licenses/by/4.0/).