In their seminal paper, Lubotzky, Phillips and Sarnak (LPS) defined the notion of regular Ramanujan graphs and gave an explicit construction of infinite families of $(p+1)$-regular Ramanujan Cayley graphs, for infinitely many primes $p$. In this paper we extend the work of LPS and its successors to bigraphs (biregular bipartite graphs), in several aspects: we investigate the combinatorial properties of various generalizations of the notion of Ramanujan graphs, define a notion of Cayley bigraphs, and give explicit constructions of infinite families of $(p^3+1,p+1)$-regular Ramanujan Cayley bigraphs, for infinitely many $p$. Both the LPS graphs and our ones are arithmetic, arising as quotients of Bruhat-Tits trees by congruence subgroups of arithmetic lattices in a $p$-adic group, $PGL_2(\mathbb{Q}_p)$ for LPS and $PU_3(\mathbb{Q}_p)$ for us. In both cases the Ramanujan property relates to the Ramanujan Conjecture (RC) on the respective groups. But while for $PGL_2$ the RC holds unconditionally, this is not so in the case of $PU_3$. We find explicit cases where the RC does and does not hold, and use this to construct arithmetic non-Ramanujan Cayley bigraphs as well, and prove that nevertheless they satisfy the Sarnak-Xue density hypothesis. On the combinatorial side, we present a pseudorandomness characterization of Ramanujan bigraphs, and a more general notion of biexpanders. We show that our Ramanujan bigraphs exhibit the cutoff phenomenon with bounded window size for non-backtracking random walks, either as a consequence of the Ramanujan property, or of the Sarnak-Xue density hypothesis. Finally, we present some other applications of our work: golden gates for $PU_3$, Ramanujan and non-Ramanujan complexes of type $\widetilde{A}_2$, optimal strong approximation for $p$-arithmetic subgroups of $PSU_3$ and vanishing of first Betti numbers of Picard modular surfaces.