We have found a remarkable increase (up to 60%) of the dielectric constant with the onset of magnetic order at 42 K in the metastable orthorhombic structures of YMnO 3 and HoMnO 3 that proves the existence of a strong magnetodielectric coupling in the compounds. Magnetic, dielectric, and thermodynamic properties show distinct anomalies at the onset of the incommensurate magnetic order and thermal hysteresis effects are observed around the lock-in transition temperature at which the incommensurate magnetic order locks into a temperature independent wave vector. The Mn 3+ spins and Ho 3+ moments both contribute to the magnetodielectric coupling. A large magnetodielectric effect was observed in HoMnO 3 at low temperature where the dielectric constant can be tuned by an external magnetic field resulting in a decrease of up to 8% at 7 T. By comparing data for YMnO 3 and HoMnO 3 the contributions to the coupling between the dielectric response and Mn and Ho magnetic moments are separated. The coupling between dielectric and magnetic properties recently observed in some manganites [1][2][3][4][5][6] and in other oxides 7,8 is of fundamental interest and of eminent significance for potential applications. The anomalies of dielectric (magnetic) properties at magnetic (ferroelectric) phase transitions and the possibility of tuning the dielectric constant (magnetization) by external magnetic (electric) fields open alternate perspectives in the basic understanding of the interesting materials and for the design of devices. The magnetodielectric effect can be explained by a spin-lattice coupling due to an increase of magnetic exchange energy when the magnetic ions shift their positions. 9,10 This effect is particularly strong close to or below a magnetic phase transition and may result in structural anomalies and a change of the dielectric properties.The rare earth manganites, RMnO 3 (R = rare earth metal), exhibit strong magnetic exchange interactions between the magnetic moments of the Mn 3+ ions as well as some of the magnetic R 3+ . Depending on the rare earth ionic size, RMnO 3 crystallizes in either hexagonal or orthorhombic (distorted perovskite) structure with the structural phase boundary between Ho and Dy. However, some of the hexagonal compounds can also be synthesized as a metastable phase in the orthorhombic structure by either special chemical procedures 11 or high pressure synthesis. 12 The hexagonal phases of RMnO 3 show ferroelectricity below Curie temperatures between 590 and 1000 K and antiferromagnetic (AFM) transitions below 100 K with small but distinct anomalies in the dielectric constant at or below the magnetic transitions.1-4 Since symmetry arguments do not allow a direct coupling between the Mn magnetic order and the polarization in the hexagonal structure the observed magnetodielectric coupling has to be related to secondary interactions but a microscopic explanation of these effects is not yet available. Some work has been done to investigate possible magnetodielectric effects in the orthorhombic...