In /sup 201/Tl//sup 99m/Tc dual-isotope simultaneous-acquisition (DISA) myocardial imaging, crosstalk due to Tc photons results in significant contamination of the Tl data. The objective of this work is to seek the acquisition parameters (i.e., energy window width and center) that have the optimal tradeoff between minimizing the crosstalk and maximizing the detection efficiency. The optimization criterion was based on maximizing an ideal observer signal-to-noise ratio (SNR) for the myocardial defect detection task using single-isotope and DISA projection images acquired from a torso phantom. For single-isotope images, the optimal energy windows (width/center: 26 keV/75 keV and 28 keV/165 keV for /sup 201/Tl, 30 keV/142 keV for /sup 99m/Tc) are wider than typical windows. For DISA imaging, the optimal windows varied with the /sup 99m/Tc to /sup 201/Tl activity ratio and are thus likely to depend on the uptake ratio in each patient. Using the optimal ratio 2.25-2.75 (148 MBq /sup 201/Tl and 333-407 MBq /sup 99m/Tc) with the corresponding optimal windows (22 keV/72 keV, 24 keV/167 keV, and 24 keV/140 keV) gives /sup 201/Tl images with substantially increased SNRs as well as /sup 99m/Tc images with SNRs same as those of 370 MBq /sup 99m/Tc-only images. However, without the addition of crosstalk compensation, the use of the optimal activity and energy windows alone is likely not sufficient to restore the DISA Tl SNR to that of Tl-only image.