Abstract: A search is presented for the two-body charmed baryonic decays B<em>(s)<sup>0→Λ</sup></em>c<sup>+Λc<sup>−, using a data sample collected by the LHCb experiment during 2011--2012 and 2015--2018 corresponding to an integrated luminosity of 9fb<sup>−1. The first observation of the B<em>s<sup>0→Λ</sup></em>c<sup>+Λc<sup>− decay is reported with $6.2σ$ significance, along with $4.3σ$ evidence for the B<sup>0→Λ<em>c<sup>+Λ</sup></em>c<sup>− decay. The branching fractions are measured to be B(B<sup>0→Λ<em>c<sup>+Λ</sup></em>c<sup>−)</sup></sup>=(1.01<sup>+0.27−0.28</sup>±0.08±0.15)×10<sup>−5 and B(B<em>s<sup>0→Λ</sup></em>c<sup>+Λc<sup>−)</sup></sup>=(5.0±1.3±0.5±0.8)×10<sup>−5, where the first uncertainty is statistical, the second systematic, and the third due to external inputs. These results provide novel experimental inputs for the theoretical framework describing two-body baryonic decays of B mesons via W-emission and W-exchange mechanisms.