Load transfer and mechanical strength of reinforced polymers are fundamental to developing advanced composites. This paper demonstrates enhanced load transfer and mechanical strength due to synergistic effects in binary mixtures of nano-carbon/polymer composites. Different compositional mixtures (always 1 wt% total) of multi-wall carbon nanotubes (MWNTs) and single-layer graphene (SLG) were mixed in polydimethylsiloxane (PDMS), and effects on load transfer and mechanical strength were studied using Raman spectroscopy. Significant shifts in the G-bands were observed both in tension and compression for single as well as binary nano-carbon counterparts in polymer composites. Small amounts of MWNT₀.₁ dispersed in SLG₀.₉=PDMS samples (subscripts represent weight percentage) reversed the sign of the Raman wavenumbers from positive to negative values demonstrating reversal of lattice stress. A wavenumber change from 10 cm⁻¹ in compression to 10 cm⁻¹ in tension, and an increase in elastic modulus of ~103% was observed for MWNT₀.₁SLG₀.₉=PDMS with applied uniaxial tension. Extensive scanning electron microscopy revealed the bridging of MWNT between two graphene plates in polymer composites. Mixing small amounts of MWNTs in SLG/PDMS eliminated the previously reported compressive deformation of SLG and significantly enhanced load transfer and mechanical strength of composites in tension. The orientation order of MWNT with application of uniaxial tensile strain directly affected the shift in Raman wavenumbers (2D-band and G-band) and load transfer. It is observed that the cooperative behavior of binary nano-carbons in polymer composites resulted in enhanced load transfer and mechanical strength. Such binary compositions could be fundamental to developing advanced composites such as nano-carbon based mixed dimensional systems.