Magnetoelectric materials with a large magnetoelectric response, a low operating magnetic (or electric) field, and a room‐temperature (or higher) operating temperature are of key importance for practical applications. However, such materials are extremely rare because a large magnetoelectric response often requires strong coupling between spins and electric dipoles. Herein, an example of a magnetoelectric composite is prepared by using a room‐temperature multiaxial molecular–ionic ferroelectric, tetramethylammonium tetrachlorogallate(III) (1). Investigation of the magnetoelectric effect of the magnetoelectric laminate composite indicates that its room‐temperature magnetoelectric voltage coefficient (αME) is as high as 186 mV cm−1 Oe−1 at HDC = 275 Oe and at the HAC frequency of ≈39 kHz, providing a valid approach for the preparation of magnetoelectric materials and adding a new member to the magnetoelectric material family. A magnetoelectric composite is prepared by using a room‐temperature multiaxial molecular–ionic tetramethylammonium tetrachlorogallate(III) ferroelectric. The room‐temperature magnetoelectric voltage coefficient is up to 186 mV cm−1 Oe−1 at HDC = 275 Oe and the HAC frequency is ≈39 kHz. This work demonstrates that multiaxial molecular–ionic ferroelectrics are new excellent candidates for the preparation of magnetoelectric composites.