We present the magnetotransport behavior of Li2BaSi using Boltzmann transport theory within relaxation time approximation. The semimetallic nature and anisotropic band dispersion suggest a possible large magnetoresistance. The electrical resistivities and magnetoresistance display non-saturating behavior for low magnetic field values and get saturated at higher fields due to charge-carrier uncompensation and are almost similar with and without spin-orbit coupling. Shifting the Fermi level by 0.10 eV results in tunable magnetotransport features with improved transverse MR values up to 200% for 12 T at 10 K with non-saturating behavior. Our calculations predict that this investigated compound can be deemed a better MR material for its transverse effects. © 2022 Elsevier B.V.