Typically, the search for order in grapheme-color synesthesia has been conducted by looking at the frequency of certain letter-color associations. Here, we report stronger associations when second-order similarity mappings are examined-specifically, mappings between the synesthetic colors of letters and letter shape, frequency, and position in the alphabet. The analyses demonstrate that these relations are independent of one other. More strikingly, our analyses show that each of the letter-color mappings is restricted to one dimension of color, with letter shape and ordinality linked to hue, and letter frequency linked to luminance. These results imply that synesthetic associations are acquired as the alphabet is learned, with associations involving letter shape, ordinality, and frequency being made independently and idiosyncratically. Because these mappings of similarity structure between domains (letters and colors) are similar to those found in numerous other cognitive and perceptual domains, they imply that synesthetic associations operate on principles common to many aspects of human cognition.Keywords Human associative learning . Perceptual categorization and identification . Synaesthesia . SynesthesiaAt least 1% of the population reliably associates particular colors with letters and numerals (Simner et al., 2006). Despite an explosion of research on grapheme-color synesthesia over the past two decades, little is known about how these associations are made. Why does Jane see the letter M as a deep purple, while John associates the same letter with forest green? Here we verify that there are several different sources of synesthetic associations, and we investigate both how they interact with each other and what aspects of synesthetic color they influence.To date, synesthesia research has documented a number of regularities in the grapheme-color pairs of individuals. For example, English speakers often associate the letter B with blue or brown, G with green, and so on for the first letters of other common color names (Barnett et al., 2008;Rich, Bradshaw, & Mattingley, 2005;Simner et al., 2005). Similarly, some synesthetes have adopted the colors of letter-shaped fridge magnets used in their childhoods (Witthoft & Winawer, 2006). These are regularities in first-order relations-that is, between nonrelational properties of a letter (such as its shape or name) and dimensions of synesthetic color such as hue and lightness (see also Day, 2005).A parallel line of research has begun to investigate grapheme-color pairings by looking for second-order relations, or "relations between relations." For example, letters with similar shapes, such as E and F, tend to be associated with synesthetic colors that are similar in hue (Brang, Rouw,