Behavioral research suggests two cognitive systems are at the foundations of numerical thinking: one for representing 1-3 objects in parallel and one for representing and comparing large, approximate numerical magnitudes. We tested for dissociable neural signatures of these systems in preverbal infants, by recording event-related potentials (ERPs) as 6-7.5 month-old infants (n = 32) viewed dot arrays containing either small (1-3) or large (8-32) sets of objects in a number alternation paradigm. If small and large numbers are represented by the same neural system, then the brain response to the arrays should scale with ratio for both number ranges, a behavioral and brain signature of the approximate numerical magnitude system obtained in animals and in human adults. Contrary to this prediction, a mid-latency positivity (P500) over parietal scalp sites was modulated by the ratio between successive large, but not small, numbers. Conversely, an earlier peaking positivity (P400) over occipital-temporal sites was modulated by the absolute cardinal value of small, but not large, numbers. These results provide evidence for two early developing systems of non-verbal numerical cognition: one that responds to small quantities as individual objects and a second that responds to large quantities as approximate numerical values. These brain signatures are functionally similar to those observed in previous studies of non-symbolic number with adults, suggesting that this dissociation may persist over vast differences in experience and formal training in mathematics.