The inference of Ying et al. [EPL 104, 67005 (2013)] of a composition-induced change from c-axis ordered-moment alignment in a collinear A-type AFM structure (AFMI) at small x to abplane alignment in an unknown AFM structure (AFMII) at larger x in Ca1−xSrxCo2−yAs2 with the body-centered tetragonal ThCr2Si2 structure is confirmed. Our major finding is an anomalous magnetic behavior in the crossover region 0.2 x 0.3 between these two phases. In this region the magnetic susceptibility versus temperature χ ab (T ) measured with magnetic fields H applied in the ab plane exhibit typical AFM behaviors with cusps at the Néel temperatures of ∼ 65 K, whereas χc(T ) and the low-temperature isothermal magnetization Mc(H) with H aligned along the c axis exhibit extremely soft ferromagnetic-like behaviors.Much research since 2008 has focused on studies of iron-based layered pnictides and chalcogenides due to their unique lattice, electronic, magnetic and superconducting properties [1][2][3][4][5][6]. An important family of these materials is comprised of doped and undoped bodycentered tetragonal parent compounds AFe 2 As 2 (A = Ca, Sr, Ba, Eu) with the ThCr 2 Si 2 -type structure (122-type compounds). The undoped and underdoped AFe 2 As 2 compounds exhibit a tetragonal to orthorhombic distortion of the crystal structure at T S 200 K. They also exhibit itinerant collinear antiferromagnetic (AFM) spindensity-wave ordering at a temperature T N the same or slightly lower than T S . The ordered moments in the stripe AFM structure of the orthorhombic phase are oriented in the ab plane. In 2014 a temperature Tinduced AFM spin-reorientation transition to a new AFM C 4 phase was discovered in the hole-underdoped Ba 1−x Na x Fe 2 As 2 system upon cooling below T N that can coexist with superconductivity [7]. A subsequent investigation by polarized and unpolarized neutron diffraction determined that the ordered moments in the new phase are aligned along the c axis instead of along the ab plane as in the stripe AFM structure [8]. The work on the Ba 1−x Na x Fe 2 As 2 system was followed by the observation of the same AFM C 4 phase in the Ba 1−x K x Fe 2 As 2 [9-11], Sr 1−x Na x Fe 2 As 2 [12, 13], and Ca 1−x Na x Fe 2 As 2 [14] systems. These results are important to understanding the mechanism of superconductivity and other aspects of the hole-doped iron arsenides [15][16][17][18][19][20][21].A similar but composition-induced moment realignment was suggested to occur in the isostructural CoAsbased system Ca 1−x Sr x Co 2−y As 2 [22]. CaCo 2−y As 2 has a so-called collapsed-tetragonal (cT) structure with AsAs bonding along the c axis between adjacent CoAs layers [23] and has ≈ 7% vacancies on the Co sites [24,25]. It exhibits itinerant A-type AFM ordering below T N = 52-77 K, depending on the sample, with the ordered moments of ≈ 0.3-0.4 µ B /Co (µ B is the Bohr magneton) within an ab-plane Co layer aligned ferromagnetically (FM) along the c axis and with AFM alignments between moments in adjacent Co planes [24][25][26][27][28]. The domi...