Grapheme–color synesthesia is a perceptual phenomenon where single graphemes (e.g., the letter “E”) induce simultaneous sensations of colors (e.g., the color green) that were not objectively shown. Current models disagree as to whether the color sensations arise from increased short-range connectivity between anatomically adjacent grapheme- and color-processing brain structures or from decreased effectiveness of inhibitory long-range connections feeding back into visual cortex. We addressed this issue by examining neural synchrony obtained from EEG activity, in a sample of grapheme–color synesthetes that were presented with color-inducing versus non-color-inducing graphemes. For color-inducing graphemes, the results showed a decrease in the number of long-range couplings in the theta frequency band (4–7 Hz, 280–540 msec) and a concurrent increase of short-range phase-locking within lower beta band (13–20 Hz, 380–420 msec at occipital electrodes). Because the effects were both found in long-range synchrony and later within the visual processing stream, the results support the idea that reduced inhibition is an important factor for the emergence of synesthetic colors.