Let G be a locally compact group satisfying some technical requirements and G its unitary dual. Using the theory of twisted crossed product C * -algebras, we develop a twisted global quantization for symbols defined on G × G and taking operator values. The emphasis is on the representation-theoretic aspect. For nilpotent Lie groups, the connection is made with a scalar quantization of the cotangent bundle T * (G) and with a Quantum Mechanical theory of observables in the presence of variable magnetic fields. * 2010 Mathematics Subject Classification: Primary 81S30, 47G30, Secondary 22D10, 22D25.The present article generalizes the twisted pseudo-differential operators from the Abelian case [14] to non-commutative phase space. The main obstacle is the fact that, when G is not Abelian, the unitary dual G is no longer a group. It still has a a natural (but complicated) measure theory with respect to which a non-commutative version of Plancherel theorem holds. The cohomological twisting will be shown to be possible in this context.On the other hand, we also extend the highly non-commutative formalism introduced in [16] to the presence of a group 2-cocycle. The constructions in [16] have been predated by the intensive study of pseudo-differential operators on particular types of non-commutative Lie groups, as compact or nilpotent. We cite the articles [5,7,20,21] and the books [6,19]; they contain many other relevant references.The present setting of second countable unimodular type I groups is quite general (besides compact and nilpotent, it contains the Abelian, exponentially solvable or semisimple groups, motion groups and certain discrete groups). In particular, some of them do not possess a Lie structure. Hopefully, in some subsequent publication, we will restrict to smaller classes of groups allowing a deeper analytical investigation, involving more realistic spaces of functions. For G = R n and for magnetic-type cocycles this has been undertaken in [11,12] and spectral results for magnetic Hamiltonians are contained in [14].Let us describe the content. We start exposing briefly the C * -algebraic formalism of twisted crossed products and its representation theory. The standard version can be found in [2,17]. Actually we present a modified version, containing a parameter τ connected to ordering issues. Then we recall some basics things about the cohomology of groups G with coefficients in an Abelian Polish group U . The most interesting case is U = C(G, T), the group of continuous functions on the locally compact group G with values in the torus; it is related with the unitary multipliers of the C * -algebras we deal with. We describe 2-cocycles and their pseudo-trivializations which are related, in the case of R n , with vector potentials corresponding to a given magnetic field.We go on with concrete realizations of the crossed products. We consider C * -algebras composed of functions which are bounded and uniformly continuous over G and invariant under translations. Compatible data are defined as couples (A, γ)...