We report 31 P-and 75 As-NMR studies on (Ca 4 Al 2 O 6 )Fe 2 (As 1−x P x ) 2 with an isovalent substitution of P for As. We present the novel evolution of emergent phases that the nodeless superconductivity (SC) in 0 x 0.4 and the nodal one around x = 1 are intimately separated by the onset of a commensurate stripe-type antiferromagnetic (AFM) order in 0.5 x 0.95, as an isovalent substitution of P for As decreases a pnictogen height h P n measured from the Fe plane. It is demonstrated that the AFM order takes place under a condition of 1.32Å h P n 1.42Å, which is also the case for other Fe pnictides with the Fe 2+ state in (FeP n) − layers. This novel phase evolution with the variation in h P n points to the importance of electron correlation for the emergence of SC as well as AFM order.High-transition-temperature (T c ) superconductivity (SC) in iron (Fe) pnictides (P n) 1 emerges when a stripe-type antiferromagnetic (AFM) order accompanied by a structural phase transition is suppressed by either a carrier doping, an application of pressure, etc. The parent compounds are AFM semimetal characterized by an average iron valence Fe 2+ in (FeP n) − layer separated by various block layers. These compounds are LnFeAsO ("1111") (Ln = rare earth), 1-3 AeFe 2 As 2 ("122") (Ae = Alkaline earth), 4,5 and (Ae 4 M 2 O 6 )Fe 2 As 2 ("42622"). 6-8 By contrast, the onset of AFM order has not yet been reported in Fe-phosphorus parent compounds with the Fe 2+ in the (FeP) − layer. Although the parent compound NaFeAs ("111") exhibits an AFM order, 9-11 whereas a fully gapped or nodeless SC emerges in LiFeAs without any carrier doping. 12-15 Meanwhile, the isovalent substitution of P for As in BaFe 2 (As 1−x P x ) 2 [hereafter denoted as Ba122(As, P)] brings about the SC with nodal gap. [16][17][18][19] Thus, the compounds with the Fe 2+ state in (FeP n) − layers undertake an intimate evolution into either the nodeless SC in LiFeAs and (Ca 4 Al 2 O 6 )Fe 2 As 2 20 or the nodal SC in Ba122(As,P) without any change in the valence condition of the Fe 2+ in the (FeP n) − layer. To gain further insight into a novel phase evolution when the Fe 2+ state is kept in the (FeP n) − layer, we have dealt with (Ca 4 Al 2 O 6 )Fe 2 (As 1−x P x ) 2 (hereafter denoted as Al-42622(As,P)) in which the Fe 2+ state is expected irrespective of the P substitution for As in the (FeP n) − layer separated by a thick perovskite-type block. 20,21 Here, note that a highly two-dimensional electronic structure in these compounds is in contrast with the three-dimensional one observed in Ae122(As,P)(Ae = Ba,Sr). 16,19,22 In this Letter, we report on a novel phase diagram for Al-42622(As,P) with the isovalent substitution of P for As and hence without any carrier doping. 31 P-and 75 As-NMR studies have revealed that a commensurate AFM order taking place in 0.5 x 0.95 intervenes between a nodeless SC in 0 x 0.4 and a nodal one around x = 1. We highlight that as the substitution of P for As decreases a pnictogen height h P n measured from the Fe plane, the nodeless SC...