We combine powder neutron diffraction, magnetometry and
57
Fe Mössbauer spectrometry to determine the nuclear and magnetic structures of a strongly interacting weberite-type inorganic–organic hybrid fluoride, Fe
2
F
5
(H
taz
). In this structure, Fe
2+
and Fe
3+
cations form magnetically frustrated hexagonal tungsten bronze layers of corner-sharing octahedra. Our powder neutron diffraction data reveal that, unlike its purely inorganic fluoride weberite counterparts which adopt a centrosymmetric
Imma
structure, the room-temperature nuclear structure of Fe
2
F
5
(H
taz
) is best described by a non-centrosymmetric
Ima
2 model with refined lattice parameters
a
= 9.1467(2) Å,
b
= 9.4641(2) Å and
c
= 7.4829(2) Å. Magnetic susceptibility and magnetization measurements reveal that strong antiferromagnetic exchange interactions prevail in Fe
2
F
5
(H
taz
) leading to a magnetic ordering transition at
T
N
= 93 K. Analysis of low-temperature powder neutron diffraction data indicates that below
T
N
, the Fe
2+
sublattice is ferromagnetic, with a moment of 4.1(1)
µ
B
per Fe
2+
at 2 K, but that an antiferromagnetic component of 0.6(3)
µ
B
cants the main ferromagnetic component of Fe
3+
, which aligns antiferromagnetically to the Fe
2+
sublattice. The zero-field and in-field Mössbauer spectra give clear evidence of an excess of high-spin Fe
3+
species within the structure and a non-collinear magnetic structure.
This article is part of the theme issue ‘Mineralomimesis: natural and synthetic frameworks in science and technology’.