Summary: A general optimal formulation for the dynamic Smagorinsky subgrid-scale (SGS) stress model is reported. The Smagorinsky constitutive relation has been revisited from the perspective of functional variation and optimization. The local error density of the dynamic Smagorinsky SGS model has been minimized directly to determine the model coefficient \(C_{\text S}\). A sufficient and necessary condition for optimizing the SGS model is obtained and an orthogonal condition (OC), which governs the instantaneous spatial distribution of the optimal dynamic model coefficient, is formulated. The OC is a useful general optimization condition, which unifies several classical dynamic SGS modelling formulations reported in the literature. In addition, the OC also results in a new dynamic model in the form of a Picard's integral equation. The approximation tensorial space for the projected Leonard stress is identified and the physical meaning for several basic grid and test-grid level tensors is systematically discussed. Numerical simulations of turbulent Couette flow are used to validate the new model formulation as represented by the Picard's integral equation for Reynolds numbers ranging from 1500 to 7050 (based on one half of the velocity difference of the two plates and the channel height). The relative magnitudes of the Smagorinsky constitutive parameters have been investigated, including the model coefficient, SGS viscosity and filtered strain rate tensor. In general, this paper focuses on investigation of fundamental mathematical and physical properties of the popular Smagorinsky constitutive relation and its related dynamic modelling optimization procedure.