The aim of this study was to conduct a review of the literature to assess the relationship between quantity and pattern of sucrose use and dental caries. Using hand and electronic methods (MEDLINE, EMBASE) the literature was searched for epidemiological papers concerning any relationship of sugars and dental caries published since 1856. Superficial hand searching was carried out between 1856 and 1940, detailed hand searching 1940–1966 and electronic 1966–2007. Selection criteria were set based on, but not confined to, Cochran style standards. Investigations were categorized as A, fulfilling all criteria; B1, relevant fulfilling 19 of 23 criteria; B2, relevant but fulfilling only between 12 and 18 of the selection criteria; and C, all other papers. There were 95 papers meeting most (more than 12) or all of the selected criteria. Only 1 paper was graded A; 31 as B1. There were in addition some 65 as B2 and all the rest as C, which were discarded. There were a wide variety of study designs and those graded A or B1 comprised 23 ecological cross-sectional, 7 cohort and 2 case control studies. Summary results showed that 6 papers found a positive, significant relationship of sugar quantity to dental caries, 19 of 31 studies reported a significant relationship of sugar frequency of use to dental caries. The balance of studies does not demonstrate a relationship between sugar quantity, but a moderately significant relationship of sugar frequency to dental caries.