A large room‐temperature magnetoelectric response is crucial for the practical application of magnetoelectric materials. However, such a response has never been achieved in molecular–ionic ferroelectric‐based laminated magnetoelectric composites. Herein, the laminated magnetoelectric composite of Metglas/1 (1 = [N(CH3)4][GaBrCl3] and Metglas = an amorphous FeBSi alloy) is prepared by combining the molecular–ionic ferroelectric 1 with Metglas in the longitudinally magnetized and transversely poled (L–T) mode. The room‐temperature magnetoelectric response of the composite is up to 8.74 V Oe−1 cm−1 at the resonance frequency (≈45 kHz), representing the largest room‐temperature magnetoelectric response reported for the molecular–ionic ferroelectric‐based laminated magnetoelectric composites to date.