Transition metal chalcogenides have gained significant attention for their optoelectronic and electrical applications in various fields due to their elemental composition-dependent tunable properties. Here, a facile microwave-assisted approach was used to synthesize different CuSe1–xTe1+x-based nanomaterials. By varying the Se and Te concentrations, the morphology of CuSe1–xTe1+x was tuned from nanosheet-based flowers to nanospheres. With the increase in the value of the Te-to-Se content ratio, the material shows the transition from mixed nanosheets/nanospheres to pure nanospheres, where the average sheet thickness and sphere diameter are ∼25 and 80 nm, respectively. The as-synthesized material shows high crystallinity with mixed phases of hexagonal Cu2Te and CuSe. The chemical bonding of the material exhibits shifts of the spectra toward lower binding energies with the decrease in the Se-to-Te ratio. The material exhibits a change in the absorption edge with a blue shift of the optical bandgap for the increase of the Te content. The increment in the absorption makes them eligible for solar cell application. The photoluminescence spectra of different CuSeTe samples show broad emission in the 550–950 nm range with a peak at ∼700 nm. Such optical properties enable CuSeTe materials for possible applications in optoelectronic devices. The dielectric measurement of the sample exhibits an increase in the dielectric constant and loss with temperature, whereas a decrease in both the values is apparent for increase in the frequency. The dielectric study of the material reveals its potential application for energy storage. The photo-response study demonstrated that the material can be employed for photodetector application.