Gamma camera imaging, including single photon emission computed tomography (SPECT), is crucial for research, diagnostics, and radionuclide therapy. Gamma cameras are predominantly based on arrays of photon multipliers tubes (PMTs) that read out NaI(Tl) scintillation crystals. In this way, standard gamma cameras can localize ɣ-rays with energies typically ranging from 30 to 360keV. In the last decade, there has been an increasing interest towards gamma imaging outside this conventional clinical energy range, for example, for theragnostic applications and preclinical multi-isotope positron emission tomography (PET) and PET-SPECT. However, standard gamma cameras are typically equipped with 9.5mm thick NaI(Tl) crystals which can result in limited sensitivity for these higher energies. Here we investigate to what extent thicker scintillators can improve the photopeak sensitivity for higher energy isotopes while attempting to maintain spatial resolution. Using Monte Carlo simulations, we analyzed multiple PMT-based configurations of gamma detectors with monolithic NaI (Tl) crystals of 20 and 40mm thickness. Optimized light guide thickness together with 2-inch round, 3-inch round, 60×60 mm2 square, and 76×76 mm2 square PMTs were tested. For each setup, we assessed photopeak sensitivity, energy resolution, spatial, and depth-of-interaction (DoI) resolution for conventional (140keV) and high (511keV) energy ɣ using a maximum-likelihood algorithm. These metrics were compared to those of a "standard" 9.5mm-thick crystal detector with 3-inch round PMTs. Estimated photopeak sensitivities for 511keV were 27% and 53% for 20 and 40mm thick scintillators, which is respectively, 2.2 and 4.4 times higher than for 9.5mm thickness. In most cases, energy resolution benefits from using square PMTs instead of round ones, regardless of their size. Lateral and DoI spatial resolution are best for smaller PMTs (2-inch round and 60×60 mm2 square) which outperform the more cost-effective larger PMT setups (3-inch round and 76×76 mm2 square), while PMT layout and shape have negligible (<10%) effect on resolution. Best spatial resolution was obtained with 60×60 mm2 PMTs; for 140keV, lateral resolution was 3.5mm irrespective of scintillator thickness, improving to 2.8 and 2.9mm for 511keV with 20 and 40mm thick crystals, respectively. Using the 3-inch round PMTs, lateral resolutions of 4.5 and 3.9mm for 140keV and of 3.5 and 3.7mm for 511keV were obtained with 20 and 40mm thick crystals respectively, indicating a moderate performance degradation compared to the 3.5 and 2.9mm resolution obtained by the standard detector for 140 and 511keV. Additionally, DoI resolution for 511keV was 7.0 and 5.6mm with 20 and 40mm crystals using 60×60 mm2 square PMTs, while with 3-inch round PMTs 12.1 and 5.9mm were obtained. Depending on PMT size and shape, the use of thicker scintillator crystals can substantially improve detector sensitivity at high gamma energies, while spatial resolution is slightly improved or mildly degraded compared to standard crystals.