Combining these experimental and simulation results, we hypothesise that the "flipping" motion, possible in both the low-and high-temperature phases, may in fact be the primary motion responsible for scrambling the orientation of the NH4 + cations in the channels, thereby causing the significant dielectric relaxation consistent with relaxor-like ferroelectricity. Our results suggest that rotational disorder may be an effective substitution for compositional disorder in designing new relaxor ferroelectric framework materials. While further studies of other framework materials known to exhibit significant dielectric relaxation are required to confirm if such rotational disorder is common to these if this is the case it highlights a new route to relaxor ferroelectrics that is inherently linked to these being molecular materials. Establishing this as a design criteria and how different extents and forms of rotational disorder affect the extent of dielectric relaxation should pave the way towards next-generation relaxor ferroelectrics.