The short-lived 26 Al radionuclide is thought to have been admixed into the initially 26 Al-poor protosolar molecular cloud before or contemporaneously with its collapse. Bulk inner Solar System reservoirs record positively correlated variability in mass-independent 54 Cr and 26 Mg*, the decay product of 26 Al. This correlation is interpreted as reflecting progressive thermal processing of infalling 26 Al-rich molecular cloud material in the inner Solar System. The thermally unprocessed molecular cloud matter reflecting the nucleosynthetic makeup of the molecular cloud before the last addition of stellar-derived 26 Al has not been identified yet but may be preserved in planetesimals that accreted in the outer Solar System. We show that metal-rich carbonaceous chondrites and their components have a unique isotopic signature extending from an inner Solar System composition toward a 26 Mg*-depleted and 54 Cr-enriched component. This composition is consistent with that expected for thermally unprocessed primordial molecular cloud material before its pollution by stellar-derived 26 Al. The 26 Mg* and 54 Cr compositions of bulk metal-rich chondrites require significant amounts (25-50%) of primordial molecular cloud matter in their precursor material. Given that such high fractions of primordial molecular cloud material are expected to survive only in the outer Solar System, we infer that, similarly to cometary bodies, metal-rich carbonaceous chondrites are samples of planetesimals that accreted beyond the orbits of the gas giants. The lack of evidence for this material in other chondrite groups requires isolation from the outer Solar System, possibly by the opening of disk gaps from the early formation of gas giants. molecular cloud | outer Solar System | metal-rich chondrites | isotopes | chondrite accretion regions L ow-mass stars like our Sun form by the gravitational collapse of the densest parts of molecular clouds comprising stellarderived dust and gas. Collapsing clouds swiftly evolve into deeply embedded protostars that rapidly accrete material from their surrounding envelopes via a protoplanetary disk (1), in which planetesimals and planetary embryos form over timescales of several million years (2). Chondritic meteorites (chondrites) are fragments of early-formed planetesimals that avoided melting and differentiation and, therefore, provide a record of the earliest evolutionary stages of the Sun and its protoplanetary disk. Most chondrites contain calcium−aluminum-rich inclusions (CAIs) and chondrules, which formed by high-temperature processes that included evaporation, condensation, and melting during short-lived heating events (3). CAIs represent the oldest dated solids and, thus, define the age of the Solar System at 4,567.3 ± 0.16 Ma (4). It is inferred that CAIs formed near the proto-Sun during a brief time interval (<0