Attitude estimation methods provide modern consumer, industrial, and space systems with an estimate of a body orientation based on noisy sensor measurements. The gradient descent algorithm is one of the most recent methods for optimal attitude estimation, whose iterative nature demands adequate adjustment of the algorithm parameters, which is often overlooked in the literature. Here, we present the effects of the step size, the maximum number of iterations, and the initial quaternion, as well as different propagation methods on the quality of the estimation in noiseless and noisy conditions. A novel figure of merit and termination criterion that defines the algorithm’s accuracy is proposed. Furthermore, the guidelines for selecting the optimal set of parameters in order to achieve the highest accuracy of the estimate using the fewest iterations are proposed and verified in simulations and experimentally based on the measurements acquired from an in-house developed model of a satellite attitude determination and control system. The proposed attitude estimation method based on the gradient descent algorithm and complementary filter automatically adjusts the number of iterations with the average below 0.5, reducing the demand on the processing power and energy consumption and causing it to be suitable for low-power applications.