Motivation: ASL and MRSI experiments are currently performed using different sequences, and EPI-based ASL methods suffer from spatial distortion and limited SNR. Goal(s): To develop a water unsuppressed MRSI based imaging method for high-fidelity ASL-based perfusion imaging. Approach: The SPICE sequence was integrated with a PASL module for ASL acquisition, and a GS model-based method was used for image reconstruction. Results: The proposed method achieved ASL at 2×2×2 mm3 resolution and MRSI at 2×3×3 mm3 within 9 minutes in total. Compared with typical EPI-based methods, the resulting ASL images were free from spatial distortion, and had adequate SNR within a short scan time. Impact: This work presents a new method for high-fidelity ASL-based perfusion imaging combining with MRSI-based metabolic imaging. With further development, it may provide a powerful brain imaging tool for both functional studies and clinical applications.