Dielectric responses have been investigated on the triangular-lattice antiferromagnet CuFeO2 and its site-diluted analogs CuFe1−xAlxO2 (x=0.01 and 0.02) with and without application of magnetic field. We have found a ferroelectric behavior at zero magnetic field for x=0.02. At any doping level, the onset field of the ferroelectricity always coincides with that of the noncollinear magnetic structure while the transition field dramatically decreases to zero field with Al doping. The results imply the further possibility of producing the ferroelectricity by modifying the frustrated spin structure in terms of site-doping and external magnetic field. In all these materials, the ferroelectric behavior is observed in the noncollinear magnetic phase. Katsura et al. proposed the spin current theory for the origin of ferroelectricity in the noncollinear magnetic phase [9]. In the theory, the electric dipole is induced by the spin current, which is expected to flow between noncollinear magnetic moments in analogy to the magnetic dipole induced by electric current. To produce such a ferroelectricity of magnetic origin, modification or partial lifting of spin state degeneracy may be prerequisite with use of the frustrated spin systems.Delafossite CuFeO 2 (See Fig. 1(d) for the structure) is one of candidates for such magnetic ferroelectrics. The crystal structure is characterized by the space group R3m, with two-dimensional triangular lattice layers stacked rhombohedrally along the caxis ( Fig. 1(d)). The magnetic structure of this material has been studied extensively by neutron diffraction measurements [10,11,12,13,14,15]. At zero field, a 4-sublattice collinear structure (CM-4) is observed at the lowest temperature. When the field is increased up to 7 T, a noncollinear spin structure (NC) emerges [16]. Above 12 T, a 5-sublattice collinear structure (CM-5) is realized [11]. Recently, Kimura et al. reported that the spontaneous polarization is observed in the noncollinear magnetic phase in between the 4-sublattice and 5-sublattice phases [18]. Similarly to the magnetic field, Al doping is known to easily modify the magnetic structure [13]. The 2 % substitution of Fe with Al induces the transition from CM-4 to NC at zero field and low temperature [12]. To clarify the relation between the magnetic structure and dielectric properties, the search for electric polarization is desirable also for the Al-doped crystals. In this work, we report the finding of ferroelectricity in the noncollinear magnetic phase of the Al doped crystal even in the absence of external magnetic field as well as the systematic evolution of the magneto-electric phase with Al-doping. This ensures the close relation between the noncollinear magnetic structure and ferroelectricity.Single crystals of CuFe 1−x Al x O 2 (x=0.00, 0.01, 0.02) were prepared by a floating zone method [19]. For the measurements of pyroelectric current and dielectric constant, the crystals were cut into thin planes with the widest faces parallel to (110) plane. As the electrodes, we ...