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Uncertainty quantification is essential for robust controller synthesis to ensure stability and performance under varying conditions, parameters, and external disturbances. To reduce the conservatism in the controller design, a 'tight' description of the uncertainty is crucial. While traditional frequency-domain methods provide effective uncertainty descriptions for single-input single-output (SISO) systems, they often yield inadequate and overly conservative representations in multi-input multi-output (MIMO) settings. This paper proposes a novel measure of the uncertainty that provides a better description of the uncertainty sets for MIMO systems. Additionally, it presents a computationally efficient method for optimising the frequency-domain uncertainty set while simultaneously determining the nominal model. The method also considers the case where set-bounded noise and modelling errors are present and known. The proposed method's effectiveness is validated using comparisons with the traditional methods. Finally, high-performance robust controllers are synthesised and implemented for uncertainty sets obtained using different uncertainty quantification methods on a hybrid micro-vibration rejection platform, demonstrating improved performance and reduced conservatism for the proposed method.