Achieving balanced alignment of large language models (LLMs) in terms of Helpfulness, Honesty, and Harmlessness (3H optimization) constitutes a cornerstone of responsible AI, with existing methods like data mixture strategies facing limitations including reliance on expert knowledge and conflicting optimization signals. While model merging offers a promising alternative by integrating specialized models, its potential for 3H optimization remains underexplored. This paper establishes the first comprehensive benchmark for model merging in 3H-aligned LLMs, systematically evaluating 15 methods (12 training-free merging and 3 data mixture techniques) across 10 datasets associated with 5 annotation dimensions, 2 LLM families, and 2 training paradigms. Our analysis reveals three pivotal insights: (i) previously overlooked collaborative/conflicting relationships among 3H dimensions, (ii) the consistent superiority of model merging over data mixture approaches in balancing alignment trade-offs, and (iii) the critical role of parameter-level conflict resolution through redundant component pruning and outlier mitigation. Building on these findings, we propose R-TSVM, a Reweighting-enhanced Task Singular Vector Merging method that incorporates outlier-aware parameter weighting and sparsity-adaptive rank selection strategies adapted to the heavy-tailed parameter distribution and sparsity for LLMs, further improving LLM alignment across multiple evaluations. We release our trained models for further exploration.