In addition to its caries-promoting effect, a high-sucrose diet reduces the apposition of mineralized dentin in young rats. This study was undertaken to test whether it has a similar effect on the width of the as-yet-uncalcified matrix, predentin. Female Wistar rats were weaned at the age of 3 weeks and fed for 7 weeks with either a high-sucrose diet, a non-cariogenic raw potato starch diet, or a non-cariogenic commercial powdered rat food (for reference). The sucrose diet induced the greatest number of caries lesions. Dentin formation was smaller and the predentin zone wider in rats fed a sucrose diet when compared with rats fed the reference diet. In rats fed a starch diet, dentin formation was smaller than in rats fed a reference diet, but no alterations in the areas of caries lesions or predentin width were observed. Widening of the predentin zone in rats fed a high-sucrose diet may reflect changes in odontoblast function, such as reduced matrix synthesis and possibly disturbed mineralization. Dentinal caries progression may thus be modulated by odontoblast function, not as much by matrix formation but rather by mineralization.