Accurately estimating single-axis rotational angle changes is crucial in many high-tech domains. However, traditional angle measurement techniques are often constrained by sensor limitations and environmental interferences, resulting in significant deficiencies in precision and stability. Moreover, current methodologies typically rely on fixed-axis rotation models, leading to substantial discrepancies between measured and actual angles due to axis misalignment. To address these issues, this paper proposes an innovative method for single-axis rotational angle estimation. It introduces a calibration technique for installation errors between inertial measurement units and the overall measurement system, effectively translating dynamic rotational inertial outputs to system enclosure outputs. Subsequently, the method employs triaxial accelerometers combined with zero-velocity detection technology to estimate the rotation axis position. Finally, it delves into analyzing the relationship between quaternion and axis–angle, aimed at reducing noise interference for precise rotational angle estimation. Based on this proposed methodology, a Low-Cost, a High Accuracy Measurement System (HAMS) integrating sensor fusion was designed and implemented. Experimental results demonstrate static measurement errors below ±0.15° and dynamic measurement errors below ±0.5° within a ±180° range.