Blockchain and smart contracts are one of the key technologies promoting Web 3.0. However, due to security considerations and consistency requirements, smart contracts currently only support simple and deterministic programs, which significantly hinders their deployment in intelligent Web 3.0 applications. To enhance smart contracts intelligence on the blockchain, we propose SMART, a plug-in smart contract framework that supports efficient AI model inference while being compatible with existing blockchains. To handle the high complexity of model inference, we propose an on-chain and off-chain joint execution model, which separates the SMART contract into two parts: the deterministic code still runs inside an on-chain virtual machine, while the complex model inference is offloaded to off-chain compute nodes. To solve the non-determinism brought by model inference, we leverage Trusted Execution Environments (TEEs) to endorse the integrity and correctness of the off-chain execution. We also design distributed attestation and secret key provisioning schemes to further enhance the system security and model privacy. We implement a SMART prototype and evaluate it on a popular Ethereum Virtual Machine (EVM)-based blockchain. Theoretical analysis and prototype evaluation show that SMART not only achieves the security goals of correctness, liveness, and model privacy, but also has approximately 5 orders of magnitude faster inference efficiency than existing on-chain solutions.