The linear instability of a surfactant-laden two-layer falling film over an inclined slippery wall is analyzed under the influence of external shear, which is imposed on the top surface of the flow. The free surface of the flow and the interface among the fluids are contaminated by insoluble surfactants. Dynamics of the fluid layers are governed by the Navier-Stokes equations, and the surfactant transport equations regulate the motion of the insoluble surfactants at the interface and free surface. Instability mechanisms are compared by imposing the external shear along and opposite to the flow direction. A coupled Orr-Sommerfeld system of equations is derived using the perturbation technique and normal mode analysis. The eigenmodes corresponding to the Orr-Sommerfeld eigenvalue problem are obtained by employing the spectral collocation method. The numerical results imply that the stronger external shear destabilizes the interface mode instability. However, a stabilizing impact of the external shear on the surface mode is noticed if the shear is imposed in the flow direction, which is in contrast to the role of imposed external shear on the surface mode for a surfactant-laden single layer falling film. Furthermore, in the presence of strong imposed shear, the overall stabilization of the surface mode by wall velocity slip for the stratified two-fluid flow is also contrary to that of the single fluid case. The interface mode behaves differently in the two zones at the moderate Reynolds numbers, and higher external shear magnifies the interfacial instability in both zones. An opposite trend is observed in the case of surface instability. Moreover, the impression of shear mode on the primary instability is analyzed in the high Reynolds number regime with sufficiently low inclination angle. Under such configuration, dominance of the shear mode over the surface mode is observed due to the weaker impact of the gravitational force on the surface instability. The shear mode can also be stabilized by applying the external shear in the counter direction of the streamwise flow. Conclusively, the extra imposed shear on the stratified two-layer falling film plays an active role in the control of the attitude of the instabilities. © 2020 Author(s).