Globally, 20% of all newborns are born with low birth weight (LBW). There is, therefore, an urgent need to expedite the delivery of high-impact, evidenced-based, and low-cost interventions such as kangaroo mother care (KMC (defined as continuous skin-to-skin care) and exclusive breastfeeding for this vulnerable group. A multinational World Health Organization (WHO)-supported consortium created and tested the impact of locally-specific and globally-informed phases of KMC care on KMC uptake/scale-up across multiple sites. Here we report on the study of KMC predictors that is nested within Amhara's KMC implementation trial in Amhara, Ethiopia. We used multivariate logistic regression phases to identify diverse predictors of KMC, skin-to-skin contact, and exclusive breastfeeding at hospital discharge and day 28 of life. We analysed data from 860 LBW newborns. At day 28, implementation period (adjusted odds ratio (aOR) = 3.2-5.0), hospital facility (aOR = 3.0-4.6), and having multiple births (aOR = 0.31) were the strongest predictors of effective KMC. Meanwhile, previous death of a newborn, type of health facility where delivery occurred, and previous LBW delivery were predictors of effective KMC at both time points. No single factor predicted KMC, skin-to-skin contact, and exclusive breastfeeding at all time points and across all implementation periods. Having multiple births was a negative predictor for skin-to-skin contact, while the implementation period and having older fathers (>29 years) were strong positive predictors for exclusive breastfeeding at both discharge and day 28. Mothers with a previous history of neonatal death and current skin-to-skin-care uptake strongly predicted exclusive breastfeeding uptake at both time points. At discharge, however, having a history of preterm birth and neonatal death strongly predicted exclusive breastfeeding uptake, while multiple current births, current very LBW newborns, and the use of standard binders decreased the likelihood of exclusive breastfeeding. To achieve the effective KMC coverage target of ≥80% in Ethiopia, KMC scale-up phases may have to consider the key predictors of KMC, EBF, and SSC to effectively target beneficiaries.