The abundant hydrophilic surface groups endow carbon-based nanoparticles (CDs) with intrinsic great dispersibility, however, the strong hydrophilicity limits the oil–water interface activity, restraining the performance in enhanced oil recovery. Developing CDs with simultaneously ultra-small sizes, high temperature and salt tolerance, as well as superior interfacial activity is of great significance. In this work, CDs with the size of 3.3 nm and excellent temperature and salt resistance were prepared by hydrothermal reaction, using citric acid (CA) and ethylenediamine (EDA) as precursors. Carboxyl ether carboxylate-6Na (APEC-6Na) was selected as the compound agent to construct carbon-based active nanofluids (CANs) with excellent oil–water and oil-solid interfacial activities. CANs can reduce the oil–water interfacial tension to 8.9 × 10-4 mN m−1, withstand a temperature up to 90°C and a salinity up to 6.3 × 104 mg·L-1. Even at the highest tolerant salinity, the underwater oil contact angle of 155° can be achieved, demonstrating excellent wettability control capability, which could be attributed to the synergistic effect of the compound CANs system. The increase of the contact angle of underwater oil droplets facilitates the coalescence of oil film on the lipophilic surface to form oil droplets. The electrostatic repulsion generated by the adsorption of CDs and APEC-6Na at the oil–water interface and rock surface makes the coalesced oil droplets more easily detached from the rock surface, and the oil film reduction rate exceeds 97.7 % within 24 h. The excellent oil–water and oil-solid interface properties and the structural separation pressure endows CANs with remarkable performance in core displacement experiments. Compared with simulated formation water, CANs can improve the recovery rate by 26.3 %, exhibiting important application value for improving the recovery rate of ultra-low permeability reservoirs.