In magnetically controllable ferroelectrics 1-3 , electric polarization is induced by charge redistribution or lattice distortions that occur to minimize the energy associated with both the magnetic order and interaction of spins with an applied magnetic field. Conventional approaches to designing materials that exploit such spin-mediated behaviour have focused mainly on developing the cycloidal spin order 4,5 , and thereby producing ferroelectric behaviour through the so-called antisymmetric Dzyaloshinskii-Moriya interaction 6-8. However, engineering such spin structures is challenging. Here we suggest a different approach. Direct measurements of magnetic-field-dependent variations in the polarization of the one-dimensional organic quantum magnet, tetrathiafulvalene-p-bromanil, suggest a spin-Peierls instability has an important role in its response. Our results imply that one-dimensional quantum magnets, such as organic charge-transfer complexes, could be promising candidates in the development of magnetically controllable ferroelectric materials. A straightforward guideline for designing spin-driven ferroelectricity might be to use the symmetric interaction, simply because it is more dominant in ubiquitous magnets, rather than the antisymmetric exchange interaction (that is, the Dzyaloshinskii-Moriya interaction). In this context, the up-up-down-down (↑↑↓↓) magnetic order on the alternating (ABAB) atom sites was proposed as a promising candidate for symmetric-exchange-driven ferroelectricity 9 ; this prediction has actually been confirmed in the frustrated Ising chain system, Ca 3 Co 2−x Mn x O 6 (A = Co and B = Mn) 10 , and the f-d spin-coupled state of GdFeO 3 (A = Gd and B = Fe) 11. Moreover, there is a theoretical argument that symmetric-exchange-driven ferroelectricity can host potentially large polarization 12. This recent progress is prompting a pursuit of not only materials showing the ↑↑↓↓ order but also other clear-cut examples of symmetric-exchange-driven ferroelectricity. In the same way as one-dimensional (1D) metals with inherent lattice instability (Peierls instability) 13 , 1D Heisenberg spin-1/2 quantum magnets possess an instability to form a dimer-singlet state because of the energy gain of symmetric exchange 14,15. This is known as the spin-Peierls instability, a textbook example of spin-lattice coupling. Therefore, the spin-Peierls instability with alternating ABAB spin sites can host a polar singlet-dimer and hence is expected to provide a new mechanism for magnetically controllable ferroelectrics of symmetric-exchange origin. The organic charge-transfer salt TTF-BA (tetrathiafulvalene-p-bromanil) has been proposed as a possible candidate of this new class 16 of material, namely a ferroelectric spin-Peierls material; nevertheless, direct observations of ferroelectricity, that is, electric-field reversal of polarization, have LETTERS NATURE PHYSICS