A strain sensor was prepared by reinforcing acrylonitrile butadiene rubber (NBR)-5 parts per hundred of rubber (phr) carbon black (CBH) separately with small concentration (∼0.1phr) of reduced graphene oxide (GL), multi-walled, and carbon nanotube (NTL) via a combination of conventional solution and solid processing techniques. The interactions and the electronic properties among carbon based fillers NT, CB, G and their synergy effects (NBR-CBH-GL and NBR-CBH-NTL) were investigated by using density functional theory (DFT) modeling approach. The DFT predictions were in correspondence with the experimental results. The optimum design (NBR-CBH-GL) was found to show high curing, mechanical and improved electrical properties. On account of strain sensing performance, NBR-CBH-GL exhibited high gauge factor (GF) ∼105 at 0–40% strain, which was over 900% than NBR-CBH (GF ∼104 at 0–30% strain) and the highest reported so far. This was explained by the breaking of CB networks caused by tight NBR-G structures on straining, leading to high electrical resistance. The NBR-CBH-GL also demonstrated high stability and repeatability in the cyclic loading. In terms of applications, NBR-CBH-GL exhibited high capability for vibration detections and wearable sensing, especially for detection of human bodily motions like speeches, facial deformations, bending, and relaxation of the fingers.