Hard exclusive electroproduction of π+π- pairs off hydrogen and deuterium targets has been studied by the HERMES experiment at DESY. Legendre moments 〈P1〉 and 〈P3〉 of the angular distributions of π+ mesons in the center-of-mass frame of the pair have been measured for the first time. Their dependence on the π+π- invariant mass can be understood as being due to the interference between relative P-wave (isovector) and S-, D-wave (isoscalar) states of the two pions. The increase in magnitude of 〈P1〉 as Bjorken x increases is interpreted in the framework of generalized parton distributions as an enhancement of flavour non-singlet qq̄ exchange for larger values of x, which leads to a sizable admixture of isoscalar and isovector pion pairs. In addition, the interference between P-wave and D-wave states separately for transverse and longitudinal pion pairs has been studied. The data indicate that in the f2(1270) region at 〈Q2〉=3 GeV2 higher-twist effects can be as large as the leading-twist longitudinal component. © 2004 Published by Elsevier B.V.