Stereoregular trans-poly(dienes) with three different types of functional groups were synthesized by insertion polymerization. The functional groups are located simultaneously in the polymer backbone and at both chain ends, yielding heterotelechelic and in-chain functionalized polymers. A combination of three compatible functionalization methods allows for the syntheses of these particular polymers. Nd-(BH4)(3)center dot(THF)(3) catalyzes, after activation with MgR2, the direct copolymerization of 1,3-butadiene or isoprene with polar functionalized dienes, thus enabling the functionalization of the polymer's backbone. The use of functionalized organo-Mg compounds, e.g., (PhS-C5H10)(2)Mg, for the activation of Nd(BH4)(3)center dot(THF)(3) enables the functionalization of the initiating chain-end and quenching of the polymerization with suitable reagents; e.g., Si(OEt)(4) allows for the functionalization of the terminating chain-end.